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• The FeMnO x /S(IV) system has faster removal speed and higher adsorption capacity for As(III) compared to FeMnO x alone. • The As(III) (1079 µg/L) could be decreased to less than 10 µg/L within 10 min. • The SO 5 •− radicals generated by S(IV) acting as the driving force for the redox cycle between As(III) and Mn(II/III/IV). • The possible mechanism of As(III) oxidation and removal for the FeMnO x /S(IV) system was proposed. • The FeMnO x nanocellulose aerogel broadened the scope of FeMnO x /S(IV) system in engineering applications. Manganese (Mn)-containing composite metal adsorbents are very effective at removing arsenite (As(III)) from contaminated water, however, the low removal speed and oxidation efficiency have limited their further application. In this study, a nonhomogeneous catalytic oxidation–adsorption system was constructed by coupling iron–manganese composite oxide (FeMnO x) with sulfite (S(IV)) to enhance the recovery of oxidative capacity and accelerate the removal of As(III). Experimental results showed that the FeMnO x /S(IV) system decreased the As(III) concentration from 1079 to <10 µg/L within 10 min and almost completely oxidized As(III) to As(V). In contrast, FeMnO x alone removed only 82.4% of As(III) within 30 min, and 60.0% of the adsorbed As(III) was not oxidized. Meanwhile, the adsorption capacity of FeMnO x /S(IV) system for As(III) was considerably higher than that of the only-FeMnO x system (76.5 > 46.3 mg/g). The efficient and fast As(III) removal was attributed to the SO 5 •− radical generated by S(IV) acting as the driving force for the redox cycle between As(III) and Mn(II/III/IV). Several environmental factors (e.g., solution pH and inorganic anions) and the reusability and practicality of FeMnO x were systematically investigated, and the results further confirmed the superiority of the FeMnO x /S(IV) system in As(III) removal. In particular, the proposed FeMnO x nanocellulose aerogel effectively purified arsenic-contaminated groundwater using a fixed-bed column. Thus, FeMnO x –S(IV) coupling is very promising for the purification of arsenic-contaminated water bodies. [Display omitted] [ABSTRACT FROM AUTHOR]