The adsorption of radioactive iodine is a critical concern in nuclear safety and environmental protection due to its hazardous nature and long half-life. Covalent organic frameworks (COFs) have emerged as promising materials for capturing radioactive iodine owing to their tunable porosity, high surface area, and versatile functionalization capabilities. This review provides a comprehensive overview of the application of COFs in the adsorption of radioactive iodine. We begin by discussing the sources, properties, and hazards of radioactive iodine, as well as traditional capture techniques and their limitations. We then delve into the intrinsic structures of COFs, focusing on their porosity, conjugated frameworks, and hydrogen bonding, which are pivotal for effective iodine adsorption. The review further explores various functionalization strategies, including electron-rich COFs, flexible COFs, ionic COFs, COF nanosheets, and quasi-3D COFs, highlighting how these modifications enhance the adsorption performance. Finally, we conclude with an outlook on future research directions and potential applications, underscoring the significance of continued innovation in this field. This review aims to provide valuable insights for researchers and practitioners seeking to develop advanced materials for the efficient capture of radioactive iodine.