Abstract: Micro-electrolysis (ME) technology is investigated for improving the efficiency of removal of pentavalent antimony (Sb(V)) from the environment,. In this study, an ME system composed of scrap iron filings, waste manganese fillings, and activated carbon (Fe-Mn-C ME) was used to efficiently remove Sb(V). The results proved that, compared with conventional iron-carbon micro-electrolysis (Fe-C ME), Fe-Mn-C ME significantly enhances the removal rate of Sb(V) when the hydraulic retention time is 10-24h. The Fe-Mn flocs produced by this system were analyzed using XRD, EDS, XPS, and BET surface area analysis, which revealed that the flocs were mostly Mn-substituted FeOOH and had a relatively larger specific surface area, providing better adsorption performance. Furthermore, it was found that the removal rate of Sb(V) decreased as the iron-to-carbon mass ratio increased, while it first increased and then decreased as the manganese content increased. The reduction of Fe(III) was accelerated with an increase in the addition of manganese, leading to an increase in the concentration of Fe(II). The electron transfer and the formation of Fe(II) were facilitated by the potential difference between manganese and carbon, as well as by the formation of microcells between iron and manganese, which improved the reduction ability of Sb(V). From our thorough investigation and research, this is the first report that has proposed Fe-Mn-C ME for removing antimony. It provides a novel approach and technological support for removing Sb(V) efficiently.