The effective capture of radioiodine is vital to the development of the nuclear industry and ecological environmental protection. There is, therefore, a continuously growing research exploration in various types of solid-state materials for iodine capture. During the last decade, the potential of using macrocycle and cage-based supramolecular materials in effective uptake and separation of radioactive iodine has been demonstrated. Interest in the application of these materials in iodine capture originates from their diversified porous characteristics, abundant host-guest chemistry, high iodine affinity and adsorption capacity, high stability in various environments, facile modification and functionalization, and intrinsic structural flexibility, among other attributes. Herein, recent progress in macrocycle and cage-based solid-state materials, including pure discrete macrocycles and cages, and their polymeric forms, for iodine capture is summarized and discussed with an emphasis on iodine capture capacities, mechanisms, and design strategies.