The imino group-contained porous organic polytriphenylamine, which originated from diphenylamine and 1,3,5-tris(4-bromophenyl)benzene, was designedly synthesized though Buchwald-Hartwig coupling reaction. The basic properties including morphologies, structure and thermal stability of the resulting POPs were investigated by scanning electron microscope(SEM), thermo gravimeter analysis (TGA), 13C CP/MAS solid state NMR and Fourier transform infrared spectroscope (FTIR). The pore size distribution of POPs present uniform mesoporous of sizes less than 50nm. Scanning electron microscope images show that the resulting POPs formed as an aggregation composed of nanospheres. The POPs were employed as a physicochemical stable porous medium for removal of radioactive iodine and an iodine uptake of up to 382wt% was obtained. To our knowledge, this is one of the highest adsorption value reported to date. Based on these findings, the resulting POPs shows great potential in the removal of radioactive iodine at different states, through a green, environmentally friendly, and sustainable way.