Nitrogen-enriched porous organic polymers are promising adsorbents for iodine capture and environmental sequestration. Herein, we constructed hypercrosslinked polymers (HCPs) with dual nitrogen-rich building blocks, 2,4,6-triphenyl-1,3,5-triazine and pyrrole. The resulting polymer presented high nitrogen content up to 8.04%, surface area of 222.8 m(2) g(-1), and high thermal stability. 257 wt% iodine uptake capacity was obtained as a result of several elements such as high nitrogen contents, high porosity, and pi-electron conjugated structure of the polymer. Spectral studies demonstrated that iodine uptake could occur at triazine and pyrrole moieties combined with aromatic rings in the polymer chain and the iodine nature was polyiodide anions. In addition, the material could be efficiently recycled without significant loss of iodine uptake capacity. Our work presented promising results for HCPs as economical adsorbents for the removal of iodine and other contaminates for environmental remediation applications.