The release of carbon dioxide into the atmosphere from the combustion of fossil fuels to produce energy contributes to severe climate change. Transitioning from fossil fuels to nuclear energy, which is free of carbon emissions, presents its own set of challenges, particularly the potential release of radioactive iodine in handling nuclear waste and in the instance of a nuclear accident. The ongoing research aimed to harness the advantages of porous organic polymers to capture iodine generated during nuclear fission by synthesizing them in an environmentally friendly and cost-effective hydrothermal process. Herein, a melamine-based porous organic polymer (MPOP-4), possessing reliable thermal and chemical stability, highly porous (SABET=195.48 m2/g), designed for iodine capture, is reported. The synthesis of MPOP-4 using melamine and uracil as basic building blocks showed high iodine vapor capture capacities in various media (6.30 g/g at 80 °C, 4833.15 mg/g from aqueous solution, and 1.98 g/g at 25 °C), accompanied by good regeneration ability. A significant abundance of nitrogen content, conjugated π-electron arrangement, and porous network make it an efficient iodine adsorbent. This study suggests the green nature (metal-free) of MPOP-4 and its ability to adsorb iodine.