Radioactive pollution has become a cause of concern these days, especially with the growing industrial revolution. After traditional fossil fuels, nuclear power is important for fulfilling the growing needs of the world that leads to the release of radionuclides like uranium (235,238U), cesium (137Cs), neptunium (237Np), plutonium (239Pu), americium (241,243Am), curium (245Cm), strontium (90Sr), barium (133,140Ba), etc. that have long-term radiological and chemical toxicities, which make them hazardous even in small concentrations. They can also pollute the environment to varying degrees. They have long-term negative impacts on human health, including neurological abnormalities, birth deformities, infertility, and numerous types of cancer in different organs. Thus, there is an utmost need for the management and isolation of radioactive waste for the safety of the people and the future of the world. Phytoremediation is the process of removing contaminants from the contaminated site or making sure that the contaminants are less harmful after the process. Some of the phytoremediation approaches known to have mitigated radioactive pollutants include Phytoextraction, Phytodegradation, Phytostabilization, Phytovolatilization, Rhizofilteration, and/or a combination of these methods. A few of the plant species that have been reported for radionuclide phytoremediation include Triticum, Calotropis, Brassica, Helianthus, Catharanthus, Eichhornia, etc. Compared to existing remediation technologies, phytoremediation is more economical and environmentally beneficial. However, there are still some challenges that need to be addressed for more commercial applications of these methods such as the selection of suitable plant species, slower and long-term low performance, seasonal factors, applicability for contaminants deep in the soil, proper disposal, and management of plant due to potential chance of spread of more invasive plant species. Along with that, these approaches may face regulatory hurdles and public skepticism due to concerns about potential exposure to contaminants, negative effects on local communities and individuals near the contaminated sites, and long- term effects on the ecosystem and local biodiversity due to the risks associated with these remediation methods. Addressing these challenges will require ongoing study, technological developments, and a case-by-case assessment of phytoremediation’s feasibility for specific radioactive contaminants and environmental conditions. With ongoing research being continuously explored in this field, phytoremediation is projected to assume a growing function in the wider picture of environmental remediation, providing a sustainable and natural solution to the challenges faced by radioactive contaminants. The present study aims to present a comprehensive review exploring the pivotal role of plants in mitigating the threat of radioactive pollutants through phytoremediation elucidating its fundamental principles, mechanisms, hyperaccumulating plant species, addressing present challenges, and future research directions for phytoremediation to tackle this critical environmental concern.