This paper describes the arsenite [As(III)] removal performance of manganese oxide-coated-alumina (MOCA) and its interaction with As(III) in drinking water. MOCA was characterized by XRD, SEM, EDAX, gas adsorption porosimetry, and point of zero charge (pH(pzc)) measurements. Raman spectroscopy coupled with sorption experiments were carried out to understand the As(III) interaction with MCCA. As(III) sorption onto MOCA was pH dependent and the optimum removal was observed between a pH of 4 and 7.5. The Sips isotherm model described the experimental equilibrium data well and the predicted maximum As(III) sorption capacity was 42.48 mg g(-1), which is considerably higher than that of activated alumina (20.78 mg g(-1)). The sorption kinetics followed a pseudo-second-order equation. Based on sorption and spectroscopic measurements, the mechanism of As(III) removal by MOCA was found to be a two-step process, i.e. oxidation of As(III) to arsenate (As(V)) and retention of As(V) on MOCA surface, with As(V) forming an inner surface complex with MOCA. The results of this study indicated that MOCA is a promising alternative sorbent for As(III) removal from drinking water. (C) 2009 Elsevier B.V. All rights reserved.