The rational design of active and sustainable heterogeneous catalysts towards advanced oxidation process (AOPs) is of great significance for water remediation. Here, we synthesized Fe-0/graphitized carbon composite catalysts for efficient removal of bisphenol A (BPA) by activating peroxymonosulfate (PMS). The Fe-0/graphitized carbon composites were obtained by the pyrolysis of iron-tannic modified cotton, where tannic acid (TA) is an eco-friendly and low-cost polyphenol that can strongly form complexes with iron ions. The introduction of iron could significantly regulate the graphitization of carbon by changing the pyrolysis temperature. The combination of Fe-0 and graphitized carbon can endow Fe-TCs with an enhanced adsorption ability due to strong complexation between Fe-0 and BPA. The pyrolysis of iron-tannic modified cotton may serve as a novel strategy to design an efficient low-toxic metal-carbon catalyst for sulfate radical based processes in water remediation.