2D perovskites are recently attracting a significant amount of attention, mainly due to their improved stability compared with their 3D counterpart, e.g., the archetypical MAPbI3. Interestingly, the first studies on 2D perovskites can be dated back to the 1980s. The most popular 2D perovskites have a general formula of (RNH3)2MAn−1MnX3n+1, where n represents the number of metal halide octahedrons between the insulating organic cation layers. The optoelectronic properties of 2D perovskites, e.g., band gap, are highly dependent on the thickness of the inorganic layers (i.e., the value of n). Herein, 2D perovskites are arbitrarily divided into three classes, strict 2D (n = 1), quasi‐2D (n = 2–5), and quasi‐3D (n > 5), and research progress is summarized following this classification. The majority of existing 2D perovskites only employ very simple organic cations (e.g., butyl ammonium or phenylethyl ammonium), which merely function as the supporting layer/insulating barrier to achieve the 2D structure. Thus, a particularly important research question is: can functional organic cations be designed for these 2D perovskites, where these functional organic cations would play an important role in dictating the optoelectronic properties of these organic–inorganic hybrid materials, leading to unique device performance or applications?