The use of fossil fuels for energy production is accompanied by carbon dioxide release into the environment causing catastrophic climate changes. Meanwhile, replacing fossil fuels with carbon-free nuclear energy has the potential to release radioactive iodine during nuclear waste processing and in case of a nuclear accident. Therefore, developing efficient adsorbents for carbon dioxide and iodine capture is of great importance. Two nitrogen-rich porous polymers (NRPPs) derived from 4-bis-(2,4-diamino-1,3,5-triazine)-benzene building block were prepared and tested for use in CO2 and I2 capture. Copolymerization of 1,4-bis-(2,4-diamino-1,3,5-triazine)-benzene with terephthalaldehyde and 1,3,5-tris(4-formylphenyl)benzene in dimethyl sulfoxide at 180 °C afforded highly porous NRPP-1 (SABET = 1579 m2 g-1) and NRPP-2 (SABET = 1028 m2 g-1), respectively. The combination of high nitrogen content, π-electron conjugated structure, and microporosity makes NRPPs very effective in CO2 uptake and I2 capture. NRPPs exhibit high CO2 uptakes (NRPP-1, 6.1 mmol g-1 and NRPP-2, 7.06 mmol g-1) at 273 K and 1.0 bar. The 7.06 mmol g-1 CO2 uptake by NRPP-2 is the second highest value reported to date for porous organic polymers. According to vapor iodine uptake studies, the polymers display high capacity and rapid reversible uptake release for I2 (NRPP-1, 192 wt % and NRPP-2, 222 wt %). Our studies show that the green nature (metal-free) of NRPPs and their effective capture of CO2 and I2 make this class of porous materials promising for environmental remediation.