The efficient and selective capture of iodine is indispensable for the sustainable production of nuclear energy and radiation therapy. Herein we are reporting the ultrafast synthesis of triazine tryptophan-derived mesoporous polymer (average pore size of ∼3 nm) containing functional amine and imine groups, embedded within a π-rich system via triazolinedione (TAD)− indole reactions. The mesoporous network shows excellent chemical stability against a wide range of regular solvents and thermal stability up to 250 °C. The polymer can efficiently adsorb iodine in different media, including in the vapor phase and organic phase and in water. The equilibrium iodine adsorption capacity is reported as 3.9 g g −1 in the vapor phase, 1.5 g g −1 in the organic phase (n-hexane), and 2.8 g g −1 in the aqueous phase. Further, their applicability in different types of real-world water matrixes such as tap water, river water, lake water, sewage treatment plant water, and seawater is also successfully tested. Finally, column chromatographic experiments revealed that the material is useful for capturing iodine in dynamic closed systems without losing efficiency.