Organic pollutants produced during industrial production are putting more stress on natural water resources. It is a considerable challenge to realize water remediation from organic pollutants in a cost-effective way. Here, we report a feasible method to fabricate Fe3N-decorated porous carbon frameworks (F/M-Fe) by one-step pyrolysis of wheat flour, melamine and metal ions. The prepared F/M-Fe possessing intrinsic peroxidase (POD)- and catalase (CAT)-like activities could effectively remove organic pollutants, which could be deduced from the degradation of methylene blue trihydrate (MB), rhodamine B (RhB), and tetracycline (TC) as pollutant simulants, as well as excess H2O2 without consuming additional resources and energy. The degradation process was facilitated by the primary active intermediates of ˙OH and 1O2 in the catalytic pathway, with efficiencies of 95.8% for MB, 91.6% for RhB, and 92.3% for TC achieved within 10, 50, and 70 min, respectively. Thanks to the encouraging recycling behavior and well-conditioned tolerance, F/M-Fe shows satisfactory catalytic performance on a proof-of-concept filter-type device for MB degradation. In addition, F/M-Fe could reduce organic pollutants to a safe level, under which zebrafish can survive well, which exhibited the potential value of F/M-Fe in water remediation.