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The efficient capture and storage of radioactive iodine (¹²⁹I or ¹³¹I), which can be formed during nuclear energy generation or nuclear waste storage, is of paramount importance. Herein, we present highly efficient aerogels for reversible iodine capture, namely, porous silsesquioxane–imine frameworks (PSIFs), constructed by condensation of octa(3-aminopropyl)silsesquioxane cage compound and selected multitopic aldehydes. The resulting PSIFs are permanently porous (Brunauer–Emmet–Teller surface areas up to 574 m²/g), thermally stable, and present a combination of micro-, meso-, and macropores in their structures. The presence of a large number of imine functional groups in combination with silsesquioxane cores results in extremely high I₂ affinity with uptake capacities up to 485 wt %, which is the highest reported to date. Porous properties can be controlled by the strut length and rigidity of linkers. In …