Advanced Materials

The separation of xylene isomers, especially para‐xylene, is a crucial but challenging process in the chemical industry due to their similar molecular dimensions. Here, a flexible metal–organic framework, Ni(ina)2, (ina = isonicotinic acid) is employed to effectively discriminate xylene isomers. The adsorbent with adaptive deformation accommodates the shapes of isomer molecules, thereby translating their subtle shape differences into characteristic framework deformation energies. Through a combination of multiple local flexibility behaviors, Ni(ina)2 exhibits guest‐specific structural transformations that energetically favor para‐xylene over other isomers. Single‐crystal X‐ray diffraction, in situ powder X‐ray diffraction, and theoretical investigations validate this “adaptive fitting” mechanism, where the degree of structural deformation scales with the mismatch between the molecular shape and pore geometry. As a result, Ni(ina)2 achieves exceptional para‐xylene selectivity in both liquid and vapor phase separations, maintaining a high para‐xylene purity and productivity. This work demonstrates a novel strategy of exploiting framework flexibility to address challenging molecular separations and provides fresh insights into the design of selective adsorbents.

High‐performance bifunctional electrocatalyst for oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is the keystone for the industrialization of rechargeable zinc‐air battery (ZAB). In this work, the modulation in the spin state of Fe single atom on nitrogen doped carbon (Fe1‐NC) is devised by Co3O4 (Co3O4@Fe1‐NC), and a mediate spin state is recorded. Besides, the d band center of Fe is downshifted associated with the increment in eg filling revealing the weakened interaction with OH* moiety, resulting in a boosted ORR performance. The ORR kinetic current density of Co3O4@Fe1‐NC is 2.0‐ and 5.6 times higher than Fe1‐NC and commercial Pt/C, respectively. Moreover, high spin state is found for Co in Co3O4@Fe1‐NC contributing to the accelerated surface reconstruction of Co3O4 witnessed by operando Raman and electrochemical impedance spectroscopies. A robust OER activity with overpotential of 352 mV at 50 mA cm⁻² is achieved, decreased by 18 and 60 mV by comparison with Co3O4@NC and IrO2. The operando Raman reveals a balanced adsorption of OH* species and its deprotonation leading to robust stability. The ZAB performance of Co3O4@Fe1‐NC is 193.2 mW cm⁻² and maintains for 200 h. Furthermore, the all‐solid‐state ZAB shows a promising battery performance of 163.1 mW cm⁻².

Organic mixed ionic‐electronic conductors (OMIECs) have garnered significant attention due to their capacity to transport both ions and electrons, making them ideal for applications in energy storage, neuromorphics, and bioelectronics. However, charge compensation mechanisms during the polymer redox process remain poorly understood, and are often oversimplified as single‐ion injection with little attention to counterion effects. To advance understanding and design strategies toward next‐generation OMIEC systems, a series of p‐channel carboxylated mixed conductors is investigated. Varying side‐chain functionality, distinctive swelling character is uncovered during electrochemical doping/dedoping with model chao‐/kosmotropic electrolytes. Carboxylic acid functionalized polymers demonstrate strong deswelling and mass reduction during doping, indicating cation expulsion, while ethoxycarbonyl counterparts exhibit prominent mass increase, pointing to an anion‐driven doping mechanism. By employing operando grazing incidence X‐ray fluorescence (GIXRF), it is revealed that the carboxyl functionalized polymer engages in robust cation interaction, whereas ester functionalization shifts the mechanism towards no cation involvement. It is demonstrated that cations are pivotal in mitigating swelling by counterbalancing anions, enabling efficient anion uptake without compromising performance. These findings underscore the transformative influence of functionality‐driven factors and side‐chain chemistry in governing ion dynamics and conduction, providing new frameworks for designing OMIECs with enhanced performance and reduced swelling.

Electromagnetic interference (EMI) shielding materials with low electromagnetic (EM) waves reflection characteristics are ideal materials for blocking EM radiation and pollution. Materials with low reflectivity must be constructed using materials with excellent EM waves absorption properties. However, materials simultaneously possessing both low reflectivity and excellent EMI shielding performance remain scarce, consequently, multilayer structures need to be developed. Poly(p‐phenylene–2,6–benzobisoxazole) nanofibers (PNF) are prepared by deprotonation. PNF are combined with MXene and heterostructure MXene@Ni prepared by in‐situ growth; MXene@Ni/PNF acts as an EM absorption layer while MXene/PNF acts as an EM reflective layer. Finally, (MXene@Ni/PNF)–(MXene/PNF) aerogels are prepared by layer‐by‐layer freeze‐drying based on the layered modular design concept. Experimental characterizations revealed that (MXene@Ni/PNF)–(MXene/PNF) aerogels enable the efficient absorption‐reflection‐reabsorption of EM waves, effectively eliminating EMI. When the mass ratio of MXene to Ni in MXene@Ni is 1:6 and the mass fraction of MXene in the reflective layer is 80 wt.%, the (MXene@Ni/PNF)–(MXene/PNF) aerogels exhibit excellent EMI shielding performance (71 dB) and a very low reflection coefficient (R = 0.10). Finite element simulations verified that the developed asymmetric structural aerogels achieve high EMI shielding performance with low reflection characteristics. In addition, (MXene@Ni/PNF)–(MXene/PNF) aerogels display excellent infrared camouflage ability.

Material photocontrol has gained importance in process engineering and biomedical applications. However, highly photoreactive materials are intrinsically unstable to light, which limits their continuous use in lit environments owing to their gradual deterioration. Herein, synergistically photocontrollable materials in the presence of acid are developed to overcome the conventional trade‐off between their photoreactivity and photostability. Pyrenylsilicon derivatives are designed as synergistically cleavable moieties on C–Si bonds under simultaneous treatment with light and acid through photoinduced dearomatization and protonation to generate the Wheland intermediate, whereas the derivatives are highly stable to light or acid alone. The unique reactivity of pyrenylsilicon derivatives is applied to various polymer network crosslinkers, enabling synergistic control and degradation of materials with light and acids. Because of their high photostability in the absence of acids, these materials can be utilized as optical materials, robust elastomers, and 3D photoprinted gels.

The efficient adsorption‐based separation of krypton (Kr) and xenon (Xe) is of paramount importance but is challenged by their similar physicochemical properties. While carbon adsorbents are theoretically promising for Kr/Xe sieving, practical success has remained elusive. Here, a series of ultramicroporous carbon molecular sieves synthesized from sucrose‐derived hydrochar is reported. The study employs careful characterization and controlled thermal pyrolysis to tailor ultramicropore formation and elucidate the evolution of the carbon framework. The leading material, C‐Suc‐750, has an ideal pore size of ≈4.0 Å. In particular, C‐Suc‐750 has achieved a remarkable Kr/Xe uptake ratio of 39.3 at ambient conditions, setting a new benchmark for selective Kr adsorption and molecular sieving of Kr/Xe. Breakthrough experiments further confirm the superior molecular sieving performance of C‐Suc‐750, highlighting its potential for Kr recovery in nuclear waste treatment. Moreover, molecular dynamics (MD) simulations demonstrate the critical role of narrow slit‐pore of the carbon molecular sieve in molecular sieving separation of Kr/Xe, providing insights into the mechanism driving this selectivity.

Triple‐negative breast cancer has an immunologically “cold” microenvironment, which leads to resistance to current immunotherapy. The activation of stimulator of interferon genes (STING) pathway has been thought a promising strategy to enhance immunotherapy efficacy. In this study, we adopted a comprehensive strategy that integrates innate immune responses with tumor‐targeting photothermal therapy (PTT) to simultaneously tackle multiple immune‐suppressive mechanisms in breast cancer. This semiconducting polymeric nanoagonists (DPTT‐Mn Lipo NPs) mediated PTT can effectively initiate tumor cell apoptosis and induce ICD, thereby reprogramming the immunosuppressive TME and activating STING. We confirmed the modulation of the TME through the PTT‐mediated ICD effect and the transactivation of the cGAS‐STING pathway in immune cells of the TME due to the released dsDNA via ICD, such as macrophages and DCs. Indeed, DPTT‐Mn Lipo NPs‐mediated PTT promoted M1 polarization of tumor‐associated macrophages, augmented T‐cell infiltration, facilitated dendritic cell (DC) maturation, and regulated type I interferon factor secretion, leading to efficient tumor suppression. Most importantly, the combination of DPTT‐Mn Lipo NPs‐based PTT with a checkpoint blockade therapy (anti‐PD‐1) can elicit long‐term immune memory besides tumor eradication. Collectively, this nano‐system can systemically activate antitumor immunity through STING activation and potentially establish long‐term memory against tumor recurrence.

Silver bismuth disulfide (AgBiS2) colloidal nanocrystals (CNCs) have emerged as ecofriendly photoactive materials with excellent photoconductivity and high absorption coefficients, in compliance with the restriction of hazardous substances (RoHS) guidelines. To maximize the theoretical potential of AgBiS2 CNC solar cells, a new diketopyrrolopyrrole (DPP)‐based polymer, BD2FCT, optimized as a hole transport layer (HTL), is developed. This asymmetric thiophene‐rich polymer HTL effectively complements the optical absorption spectrum of CNCs and forms a homogeneous layer atop the CNCs, facilitating favorable vertical charge transfer through intrinsic molecular packing. Furthermore, the BD2FCT HTL aligns energetically with AgBiS2, significantly reducing charge recombination at the CNC/HTL interfaces and enhancing charge extraction and photocurrent generation across the entire optical absorption spectrum. These characteristics are further optimized through precise molecular engineering. Additionally, a low‐bandgap acceptor, IEICO‐4F, is structurally incorporated with the BD2FCT polymer to further improve charge funneling and complementary absorption. Transient absorption spectroscopy reveals enhanced hole transfer from CNC to BD2FCT‐29DPP:IEICO‐4F, resulting in reduced charge recombination and efficient charge extraction. Consequently, a BD2FCT‐based AgBiS2 CNC solar cell achieves a power conversion efficiency (PCE) of 10.1%, demonstrating significant improvements in short‐circuit current density (JSC) and fill factor (FF).

The heteroepitaxy of 2D materials with engineered bandgaps are crucial to broaden the spectral response for their integrated optoelectronic devices. However, it is a challenge to achieve the high‐oriented epitaxy and integration of multicomponent 2D materials with varying lattice constants on the same substrate due to the limitation of lattice matching. Here, in‐plane adaptive heteroepitaxy of a series of high‐oriented 2D cesium bismuth halide (Cs3Bi2X9, X = I, Br, Cl) single crystals with varying lattice constants from 8.41 to 7.71 Å is achieved on c‐plane sapphire with distinct lattice constant of 4.76 Å at a low temperature of 160 °C in an air ambient, benefiting from tolerable interfacial strain by switching compressive stress to tensile stress during a 30° rotation of crystal orientation. First‐principles calculation demonstrates that those are all thermodynamically stable phases, deriving from multiple minima of interfacial energy between single crystals and sapphire substrate. The detectivity of Cs3Bi2I9 photodetector reaches up to 3.7 × 10¹² Jones, deriving from high single‐crystal quality. This work provides a promising experimental strategy and basic theory to boost the heteroepitaxy and integration of 2D single crystals with varying lattice constants on low‐cost dielectric substrate, paving the way for their applications in integrated optoelectronics.

Photoelectrochemical (PEC) water splitting for hydrogen generation holds immense potential for addressing environmental and energy crises. Tailoring non‐covalent interaction via a single atom is anticipated to realize prominent hole extracting facilitating PEC performance, but it has never been reported. In this study, single atom Co‐N4 is coordinated with 5‐fluoroanthranilic acid (FAA) molecules, then used as a non‐covalent hole‐extracting layer on a BiVO4 substrate. Experiments including X‐ray absorption fine spectra, Kelvin probe force microscopy, transient absorption, and theoretical calculation demonstrate the FAA coordination alters the local configuration of the central Co atom, adjusting the interfacial non‐covalent interaction, thereby reducing the barrier of charge transfer between BiVO4 and the hole‐extracting layer. Consequently, photogenerated carriers are more effectively separated, and the PEC water oxidation performance is significantly enhanced with the photocurrent density of 5.47 mA cm⁻² at 1.23 V versus RHE, much higher than those of previously reported BiVO4 photoanodes composited with porphyrin‐based compounds. Experiments and theoretical simulation confirm that the boosted PEC performance originates from exceptional interfacial charge transfer rather than surface catalysis dynamic. This study provides an efficient strategy for tailoring non‐covalent interaction by regulating single‐atom coordination and promoting hole extract to boost PEC water oxidation activity.

Direct regeneration of spent lithium‐ion batteries presents a promising approach to effectively reuse valuable resources and benefit the environment. Unlike controlled laboratory conditions that commonly facilitate impurity purification and minimize structural damage, the LiFePO4 cathode black mass faces significant interfacial challenges, including structure deterioration, cathode‐electrolyte interphase residues, and damage from storage procedures, which hinder lithium replenishment and structure regeneration. Here, a metal‐solvent chelation reaction using a lithium acetylacetonate solution is introduced to address these challenges under ambient conditions. This method regulates the near‐surface structure through strong chelation between Acac‒ anions and Fe (III) elements, thus effectively eliminating the degraded amorphous phase and residual fluorine compounds. By direct lithium connection and reducing diffusion barriers, the reconstructed surface facilitates the re‐lithiation process. The regenerated LiFePO4 cathodes demonstrate a capacity retention of 88.5% after 400 cycles at 1 C, while also outperforming traditional recycling methods in terms of environmental and economic benefits. This approach provides a promising solution for regenerating degraded LiFePO4 cathodes from actual dismantled black mass, thereby accelerating the practical application of battery recycling.

Photodynamic therapy (PDT) is attracting widespread attention as a promising strategy for tumor treatment. However, the efficacy of PDT is severely limited by the insufficient tissue penetration depth of the light source and low reactive oxygen species (ROS) generation efficiency. Herein, the metal doping strategy is reported to construct a series of defect‐rich M‐doped amorphous CoMo‐layered double hydroxide (a‐M‐CoMo‐LDH, M = Mn, Cu, Al, Ni, Mg, Zn) photosensitizers (PSs) for NIR‐II PDT. Especially, M‐doped CoMo‐LDH nanosheets are synthesized through a simple hydrothermal method and then etched by acid treatment to prepare defect‐rich a‐M‐CoMo‐LDH nanosheets. Under NIR‐II 1270 nm laser irradiation, the defect‐rich a‐Zn‐CoMo‐LDH nanosheets exhibit the optimal PDT performance compared with other a‐M‐CoMo‐LDH nanosheets, and also possess much higher ROS production activity (3.9 times) than that of the pristine a‐CoMo‐LDH, with a singlet oxygen quantum yield up to 1.86, which is the highest among all the reported PSs. After polyethylene glycol (PEG) modification, the a‐Zn‐CoMo‐LDH‐PEG nanosheets can function as an effective inorganic PS for PDT, effectively inducing cell apoptosis in vitro and eradicating tumors in vivo. Notably, transcriptome sequencing analysis and further molecular validation highlight the critical role of the apoptotic/p53/AMPK/oxidative phosphorylation signaling pathways in a‐Zn‐CoMo‐LDH‐PEG‐induced cancer cell apoptosis.

Flexible films with optimal piezoelectric performance and water‐triggered dissolution behavior are fabricated using the co‐dissolution–evaporation method by mixing trimethylchloromethyl ammonium chloride (TMCM‐Cl), CdCl2, and polyethylene oxide (PEO, a water‐soluble polymer). The resultant TMCM trichlorocadmium (TMCM‐CdCl3) crystal/PEO film exhibited the highest piezoelectric coefficient (d33) compared to the films employing other polymers because PEO lacks electrophilic or nucleophilic side‐chain groups and therefore exhibits relatively weaker and fewer bonding interactions with the crystal components. Furthermore, upon slightly increasing the amount of one precursor of TMCM‐CdCl3 during co‐dissolution, this component gained an advantage in the competition against PEO for bonding with the other precursor. This in turn improved the co‐crystallization yield of TMCM‐CdCl3 and further enhanced d33 to ≈71 pC/N, exceeding that of polyvinylidene fluoride (a commercial flexible piezoelectric) and most other molecular ferroelectric crystal‐based flexible films. This study presents an important innovation and progress in the methodology and theory for maintaining a high piezoelectric performance during the preparation of flexible multi‐component piezoelectric crystal films.

Extracellular matrix (ECM) guides cell behavior and tissue fate. Cell populations are notoriously heterogeneous leading to large variations in cell behavior at the single‐cell level. Although insights into population heterogeneity are valuable for fundamental biology, regenerative medicine, and drug testing, current ECM analysis techniques only provide either averaged population‐level data or single‐cell data from a limited number of cells. Here, extracellular protein identification cytometry (EPIC) is presented as a novel platform technology that enables high‐throughput measurements of local nascent protein deposition at single‐cell level. Specifically, human primary chondrocytes are microfluidically encapsulated in enzymatically crosslinked microgels of 16 picoliter at kHz rates, forming large libraries of discrete 3D single‐cell microniches in which ECM can be deposited. ECM proteins are labeled using fluorescence immunostaining to allow for nondestructive analysis via flow cytometry. This approach reveals population heterogeneity in matrix deposition at unprecedented throughput, allowing for the identification and fluorescent activated cell sorting‐mediated isolation of cellular subpopulations. Additionally, it is demonstrated that inclusion of a second cell into microgels allows for studying the effect of cell‐cell contact on matrix deposition. In summary, EPIC enables high‐throughput single‐cell analysis of nascent proteins in 3D microenvironments, which is anticipated to advance fundamental knowledge and tissue engineering applications.

This paper presents a study on a novel porous polymer based on triphenylamine (LPCMP) as an excellent cathode material for lithium‐ion batteries. Through structural design and a scalable post‐synthesis approach, improvements in intrinsic conductivity, practical capacity, and redox potential in an organic cathode material is reported. The designed cathode achieves a notable capacity of 146 mAh g⁻¹ with an average potential of 3.6 V, using 70% active material content in the electrode. Additionally, through appropriate structural design, the capacity can increase to 160 mAh g⁻¹. Even at a high current density of 20 A g⁻¹ (360C), the cathode maintains a capacity of 74 mAh g⁻¹, enabling full charge within 10 s. A high specific energy density of 569 Wh kg⁻¹ (at 0.1 A g⁻¹) is combined with a very high power density of 94.5 kW kg⁻¹ (at 20 A g⁻¹ corresponding to a specific energy density of 263 Wh kg⁻¹) surpassing the power density of graphene‐based supercapacitors. It exhibits highly stable cyclic performance across various current densities, retaining almost 95% of its initial capacity after 1000 cycles at 5.5C. This work presents a significant breakthrough in developing high‐capacity, high‐potential organic materials for sustainable, high‐energy, and high‐power lithium‐ion batteries.

Metal/semiconductor superlattices represent a fascinating frontier in materials science and nanotechnology, where alternating layers of metals and semiconductors are precisely engineered at the atomic and nano‐scales. Traditionally, epitaxial metal/semiconductor superlattice growth requires constituent materials from the same family, exhibiting identical structural symmetry and low lattice mismatch. Here, beyond this conventional constraint, a novel class of epitaxial lattice‐matched metal/semiconductor superlattices is introduced that utilizes refractory hexagonal elemental transition metals and wide‐bandgap III‐nitride semiconductors. Exemplified by the Hf/AlN superlattices exhibiting coherent layer‐by‐layer epitaxial growth, cross‐plane thermionic emission is observed through current–voltage measurements accomplished for the first time in any metal/semiconductor superlattices. Further, thermoreflectance measurements reveal significant enhancement in cross‐plane Seebeck coefficients attributed to carrier energy filtering by Schottky barriers. Demonstration of artificially structured elemental‐metal/wide‐bandgap compound‐semiconductor superlattices promises to usher in new fundamental physics studies and cutting‐edge applications such as tunable hyperbolic metamaterials, quantum computing, and thermionic‐emission‐based thermoelectric and thermophotonic energy conversion devices.

2D nonlayered materials (NLMs) have garnered considerable attention due to unique surface structure and bright application prospect. However, owing to the strong interatomic forces caused by intrinsic isotropic chemical bonds in all directions, the direct synthesis of ultrathin and large area 2D NLMs remains a tremendous challenge. Here, the surface‐assisted passivation growth strategy is designed to synthesize ultrathin and large size β‐Bi2O3 crystals with the thickness down to 0.77 nm and the lateral size up to 163 µm. These results are primarily ascribed to the bonding between Se atoms and the unsaturated Bi atoms on the surface of β‐Bi2O3, resulting in the surface passivation and promoting the obtaining of ultrathin β‐Bi2O3. Strikingly, the photodetectors based on β‐Bi2O3 flakes exhibit a high photoresponsivity of 71.91 A W⁻¹, an excellent detectivity of 6.09 × 10¹³ Jones, a remarkable external quantum efficiency of 2.4 × 10⁴%, an outstanding anisotropic photodetection and excellent UV imaging capability at 365 nm. This work sheds light on the synthesis of 2D ultrathin NLMs and promotes their applications in multifunctional optoelectronics.

Emerging evidence suggests that patients with inflammatory bowel diseases (IBDs) are predisposed to psychosocial disturbances, such as depression and anxiety. Regrettably, clinical antidepressants exhibit unsatisfactory therapeutic efficacy in IBD‐associated psychosocial disturbances, primarily attributed to the inherent intestinal disorders and intricate bidirectional relationship between the gut and the brain. Herein, we report a metal–polyphenol‐based antidepressant to alleviate mental disorders in dextran sulfate sodium‐induced experimental acute colitis mice via modulating the microbiota–gut–brain axis. The antidepressant, termed CSMTC, comprises a core of melittin‐encapsulated natural antioxidant enzymes (i.e., catalase and superoxide dismutase) and a protective shell composed of tannic acid–cerium ion network. Upon oral administration to colitis mice, CSMTC can effectively restore colonic redox balance, reinforce the intestinal barrier, modulate gut microbiota composition, maintain the blood–brain barrier integrity, and regulate systemic immune responses. Notably, behavioral test results reveal that CSMTC significantly alleviates the colitis‐associated mental disorder (e.g., depression‐like behavior) via the microbiota–gut–brain axis by reducing neuroinflammation, enhancing hippocampal neural plasticity, modulating hippocampal immune responses, and restoring neurotransmitter homeostasis. This work may have implications for the development of new nanodrugs for treating inflammation‐associated complications.

The limited processability of metal‐organic frameworks (MOFs) is hindered flexibility in the manipulation of their aggregation state and applications. Therefore, achieving highly processable MOFs is of great significance but a challenging goal. Herein, a facile strategy is presented for achieving the construction of solution‐processable Mg‐based MOF, NKU‐Mg‐1, allowing for dynamic control of the aggregation state through dynamic self‐assembly (DySA) process and reversible circularly polarized luminescence (CPL) switcher modulation. Notably, micron‐sized crystals of NKU‐Mg‐1 can be readily dispersed in water to form nano‐sized colloids, triggered by the dynamic COO‐Mg coordination bonding interruption by the competitive H2O‐Mg bonding. Accordingly, the aggregation state of the colloid MOF can be readily tuned from 50–80 nm up to 1000 nm, in turn enabling control of aggregation‐dependent emission. Specially, the solid‐phase aggregation can be controlled via structural transitions between 3D NKU‐Mg‐1‐rec‐1 and 2D NKU‐Mg‐1‐rec‐2 nano‐crystals, as confirmed by 3D electron diffraction. Furthermore, benefiting from its highly dynamic tunable aggregation nature, the rational incorporation of the chiral module confers significant CPL activity (glum up to 0.01). Importantly, controllable dynamic aggregation enables reversible switching of the CPL activity by precisely regulating the aggregation states. The solution‐processable and dynamic aggregation‐tunable features endow it highly promising for applications.

A textile material that can dynamically adapt to different environments while serving as an immediate alert system for early detection of life‐threatening factors in the surroundings, not only enhances the individual's health management but also contributes to a reduction in energy consumption for space cooling and/or heating. In nature, different species have their own adaptation system to ambient temperature. Inspired by the army ant nest, herein a thermal adaptive textile known as Army ant Nest Textile (ANT) for thermal management and health monitoring is reported. This textile can promptly respond to perspiration, rapidly absorb sweat, and then transform its architecture to facilitate heat dissipation. Simultaneously, the colorimetric sensing function of ANT allows it to emulate the “site migration” behavior of the army ant nest, which empowers individuals to expeditiously identify multiple health‐related signals such as body temperature, UV radiation, and sweat pH values, and warn them to move to a secure environment, thereby effectively reducing the likelihood of physical harm. Together with its excellent scalability and biocompatibility, the ANT offers a promising direction for the development of next‐generation smart e‐textiles for personal thermal and healthcare management, while satisfying the growing demand for energy saving.

Polymer semiconductors have attracted much attention for photocatalytic hydrogen evolution, but they typically exhibit micrometer‐sized particles in water‐suspension, causing severe loss in light absorption and exciton recombination. Here a molecular nanophotocatalyst featuring a donor‐acceptor motif is presented that solution is processed via a facile stirring nanoprecipitation method assisted by hydrophilic surfactants, enabling an efficient quasi‐homogenous hydrogen evolution. In contrast to the original bulk powder (heterogeneous system), these quasi‐homogenous nanophotocatalysts exhibit significantly improved light‐harvesting, water‐wettability, and exciton dissociation, resulting in distinctly enhanced (by four‐order‐of‐magnitude) photocatalytic hydrogen evolution rate. The optimized nanophotocatalysts (4CzPN/DDBAB/SDBS) generate an outstanding hydrogen evolution rate of 116.42 mmol g⁻¹ h⁻¹ and apparent quantum yield of 30.2% at 365 nm, which are among the highest reported for single‐junction organic photocatalysts. The scalability of the quasi‐homogenous photocatalysts is further demonstrated using a flow‐based flash nanoprecipitation (FNP) processing.

Halide perovskites (HPs) have demonstrated excellent direct X‐ray detection performance. Lead‐free perovskite polycrystalline wafers have outstanding advantages in large‐area X‐ray imaging applications due to their area‐scalability, thickness‐controllability, large bulk resistivity, and ease of integration with large‐area thin film transistor arrays. However, currently lead‐free perovskite polycrystalline wafers possess low sensitivity, typically less than 1000 µC Gy⁻¹ cm⁻², which severely limits their X‐ray detection applications. Here, high‐quality and large scale polycrystalline wafers of AG3Bi2I9 (AG: aminoguanidinium) with short intercluster distances are successfully prepared using a hot‐pressing method. The wafers possess high mobility‐lifetime product of 5.66 × 10⁻³ cm² V⁻¹ and therefore achieve high X‐ray sensitivity of 2675 µC Gy⁻¹ cm⁻², which can be comparable to those of the high‐quality single crystal counterpart reported by the previous research (7.94 × 10⁻³ cm² V⁻¹ and 5791 µC Gy⁻¹ cm⁻²), and represent the best results of the currently lead‐free HP polycrystalline wafers. Besides, the wafers exhibit the X‐ray detection limit as low as 11.8 nGy s⁻¹, excellent long‐term working stability, and high spatial resolution of 5.9 lp mm⁻¹ in imaging. The findings demonstrate that AG3Bi2I9 polycrystalline wafers are feasible for high‐performance X‐ray detection and imaging system.

The nervous and immune systems are closely interconnected, and influence the onset and progress of various diseases. Accordingly, understanding the interaction of the neural system and the immune system becomes very important for the treatment of intractable diseases with the analysis of therapeutic mechanisms, such as autoimmune diseases, neurodegenerative diseases, cancers, and so on. The conventional immunomodulation treatments have been mainly carried out by drug administration, but they have suffered from systemic negative side‐effects with only limited effects on the specific disease. In this Perspective, photonic nanomaterials and devices are reviewed and discussed for digitally controlled neurostimulating photomedicine via photobiomodulation and optogenetics from the unique viewpoint of neuro‐immune cross‐talks. The prospects and perspectives to integrate photonic nanomaterials with advanced wearable and implantable healthcare devices are also provided and highlighted to revolutionize the therapeutic strategies by the interaction of neural and immune systems, and optimize the treatment protocols for futuristic digital photomedicine. This approach will revolutionize the fields of neurostimulation and immune regulation for further clinical applications.

The discovery of superconductivity in 3d transition‐metal compounds with strong magnetism is interesting but rare. Especially for Mn‐based compounds, there exist only very limited materials that show superconductivity. Here, the discovery of superconductivity is reported with an onset transition temperature up to 14.2 K in a Mn‐based material MnB4, which is the highest value among the stoichiometric Mn‐based superconductors. By applying high pressure, the continuous suppression of a weak semiconducting behavior and the occurrence of superconductivity after ≈30 GPa are found. With further increasing pressure, the superconducting transition temperature (Tc) is gradually enhanced and reaches the maximum onset transition value of ≈14.2 K at 150 GPa. The synchrotron X‐ray diffraction data reveal the unchanged monoclinic (S.G: P21/c) symmetry but an unusual crossover of the lattice parameters b and c in a certain pressure region as confirmed by the theoretical calculation. The findings show a promising way to explore high Tc superconductivity by combining the 3d‐transition metal magnetic elements and light elements.

Fabrication of complex three‐dimensional (3D) structures at nanoscale is the core of nanotechnology, as it enables the creation of various micro‐/nano‐devices such as micro‐robots, metamaterials, sensors, photonic devices, etc. Among most 3D nanofabrication strategies, the guided material assembly, an efficient bottom‐up approach capable of directly constructing designed structures from precise integration of material building blocks, possesses compelling advantages in diverse material compatibility, sufficient driving forces, facile processing steps, and nanoscale resolution. In this review, we focus on assembly‐based fabrication methods capable of creating complex 3D nanostructures (instead of periodic or 2.5D‐only structures). Recent advances are classified based on the different assembly mechanisms, i.e., assembly driven by chemical reactions, physical interactions, and the synergy of multiple microscopic interactions. The design principles of representative fabrication strategies with an emphasis on their respective advantages, e.g., structural design flexibility, material compatibility, resolution, or applications are analyzed. In the summary and outlook, existing challenges, as well as possible paths to solutions for future development are reviewed. We believe that with recent advances in assembly‐based nanofabrication strategies, 3D nanofabrication has achieved tremendous progress in resolution, material generality, and manufacturing cost, for it to make a greater impact in the near future.