Iron-based materials, especially ferrous sulfide (FeS), effectively remediate chromium pollution. However, the agglomeration of FeS reduces its reactivity to chromium. Herein, carboxymethyl cellulose stabilized ferrous [email protected] polymeric substance ([email protected]) was developed to remove hexavalent chromium (Cr(VI)) from water. [email protected] (98.00%) exhibited excellent removal efficiency of 40 mg/L Cr(VI) than those of FeS (57.35%) and CMC-FeS (68.60%). [email protected] showed good removal efficiency of Cr(VI) in wide pH range (from 4 to 9) and the co-existence of ions. FTIR and XPS results demonstrated that EPS functional group accelerated the process of adsorption and precipitation. Electrochemical results showed that [email protected] transferred electrons to Cr(VI) faster than CMC-FeS. In total, this study started from a new idea of using EPS to improve the performance of CMC-FeS, and provided a simple and effective way to remediate chromium pollution without secondary pollution.