Radioactive iodine poses a significant risk to human health, particularly with regard to reproductive and metabolic functions. Designing and developing highly efficient adsorbent materials for radioactive substances remain a significant challenge. This study aimed to address this issue by the fabricating polymeric beads containing covalent organic polymer (COP) as an effective method for removing iodine vapor. To achieve this, a COP was first synthesized via the Friedel-Crafts reaction catalyzed by anhydrous aluminum chloride. Then, COP-loaded polysulfone (PSf) (COP@PSf) and PSf beads were prepared using a phase separation method. The beads produced in this research have exhibited remarkable proficiency in adsorbing iodine vapor, showing an adsorption capacity of up to 216 wt % within just 420 min, which is higher than that of most other similar beads reported in the literature.