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The effective capture and storage of volatile molecular iodine from nuclear waste is of great significance. Covalent organic frameworks (COFs) are a class of extended crystalline porous polymers that possess unique architectures with high surface areas, long-range order, and permanent porosity. Substantial efforts have been devoted to the design and synthesis of COF materials for the capture of radioactive iodine. In this review, we first introduce research techniques for determining the mechanism of iodine capture by COF materials. Then, the influencing factors of iodine capture performance are classified, and the design principles and strategies for constructing COFs with potential for iodine capture are summarized on this basis. Finally, our personal insights on remaining challenges and future trends are outlined, in order to bring more inspiration to this hot topic of research.