Efficient,　green,　and　economical　removal　of　radioactive　iodine　(I-2)　has　drawn　worldwide　attention　for　the　safe　development　of　nuclear　energy.　Metal-organic　frameworks　(MOFs)　have　been　demonstrated　to　be　potential　candidates　for　I-2　capture.　Herein　we　report　the　synthesis　of　two　novel　isomeric　MOFs　bearing　stilbene　moieties　for　exceptionally　high　I-2　adsorption.　[Cd(hsb-2)(tsbdc)1.0.5DMF　(HSB-W8)　and　Cd(hsb-2)　(tsbdc)　(HSB-W9),　which　exhibit　two-dimensional　and　twofold　interpenetrated　three-dimensional　structures,　respectively,　have　been　assembled　from　hydrogenated　Schiff　base　ligands,　hsb-2　(1,2-bis(4＇-pyridyl-methylamino)-ethane)　and　trans-stilbene-4,4-dicarboxylate　(tsbdc),　and　Cd(NO3)(2)　by　the　diffusion　method.　Such　isomers　arise　from　the　different　conformations　of　hsb-2　ligands　controlled　by　diffusion　temperatures.　The　pi-electron-rich　stilbene　moieties　render　these　Cd-MOFs　ideal　platforms　for　capture.　The　adsorption　capacities　of　HSB-W8　and　HSB-W9　in　I-2　vapor　at　room　temperature　can　reach　up　to　2.32　and　1.92　g　g(-1),　respectively,　which　are　comparable　to　the　best-performing　MOF　materials　reported　so　far.　Furthermore,　pseudo-second-order　(PSO)　kinetic　model　analysis,　Fourier　transform　infrared　(FT-IR)　spectroscopy,　Raman　spectral　analysis,　density　functional　theory　(DFT)　calculations,　and　control　experiments　were　performed　to　shed　light　on　host-guest　interactions　and　the　iodine　adsorption　mechanism.　This　work　develops　a　rational　strategy　to　design　and　synthesise　functional　MOF　materials　for　iodine　adsorption.