High-energy demands due to globalization have led to the proliferation of nuclear technology as an alternative greener energy source to meet these demands. With this proliferation comes the release of large amounts of radionuclides into the environment. Zeolitic imidazolate frameworks (ZIFs) with tunable porous structures and numerous active sites have proved to be excellent at removing these radionuclides from various environmental media. These active sites due to the presence of functional groups allow for favorable sorptive interactions between ZIF-based materials and radionuclides. With their excellent chemical stability in refluxing organic and aqueous media, ZIFs hold a special place among metal-organic framework materials with respect to capturing various types of radionuclides. Moreover, other favorable characteristics such as high thermal stability, high framework porosities (ZIF-8 surface area as high as 1970 m² g⁻¹) and abundant functional groups, make them suitable for capturing radionuclides. In this review, recent advances in the sequestration of radionuclides with ZIFs and their derived materials (composites, derivatives) are highlighted. The challenges and prospects in this fast-growing branch of coordination chemistry are briefly discussed. This work, being the first of its kind to the best of our knowledge will serve as grounding for the future development of ZIF-based materials for radionuclide removal from the environment.