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To effectively cope with the freshwater crisis, it is imperative to develop advanced remediation materials capable of radioactive iodine capture and pathogenic microorganism inactivation, avoiding the generation of secondary pollution. Herein, cyclic tripolymerization-derived porous organic polymers (POPs) (WFMC-1 to WFMC-5) were prepared via green, rapid, and economical solid-phase synthesis using a catalytic amount of PTSA·H2O (p-toluenesulfonic acid monohydrate, PTSA·H2O). This "one stone two birds" strategy realized the bidirectional treatment of environmental pollution from both the source and the post-treatment. The ferrocene-based POP (WFMC-1) with ultrafine Fe2O3 nanoparticles formed during the polymerization could take advantage of the inherent characteristic of nuclear wastewater, presenting a satisfying peroxidase-like activity in the nuclear waste, which was enhanced under the laser stimulations. WFMC-1 with photothermal-enhanced enzymatic antibacterial capacity could not only effectively eradicate the bacteria but also possessed excellent biosafety to promote the healing of infectious wounds. Additionally, all of these five POPs could act as stable and reproducible iodine adsorbents with excellent iodine capture capacity, which could realize the rapid removal of radioactive iodine from water with almost no performance decay for at least five cycles. This general synthesis strategy provides a simple and environmentally benign method for the preparation of POPs for environmental remediation. [ABSTRACT FROM AUTHOR]