Carbothermal reduction followed by magnetic separation has been recognized as an effective recovery strategy to achieve separation of Mn and Fe from ferruginous manganese ores (Fe-Mn ores). However, it is difficult to improve the recovery of manganese more than 85% by changing carbothermic roasting reduction and magnetic separation. This work clarified the underlying reason for the poor separation with the magnetic separation process and proposed a promising process for the recovery of Fe and Mn from Fe-Mn ore. The effect of operating variables on recovery and separation of Mn and Fe from Fe-Mn ore is initially investigated during the carbothermic reduction roasting process followed by magnetic separation to reveal the underlying reason for the poor separation from Fe-Mn ores. Then, the stepwise reduction behaviors of the MnO-Fe2O3 and MnO-Fe2O3-Al2O3 systems were investigated to clarify that the formation of composite oxide Mn1-xFexO (0 < x < 0.497) and hercynite (FeO center dot Al2O3) directly caused the poor separation of Fe and Mn from high-alumina Fe-Mn ores. Then, the stepwise reduction roasting behaviors of Mn1-xFexO and FeO center dot Al2O3 were investigated by XRD, SEM-EDS and XPS analysis. After adjusting the experimental parameters, iron-rich products with a Fe recovery of 94.31% and a grade of 85.21% and manganese-rich product with a Mn recovery of 90.05% and a grade of 54.35% are obtained. The mass ratio of Mn/Fe increased to 8.5 in the manganese-rich product. (C) 2019 The Society of Powder Technology Japan. Published by Elsevier B.V. and The Society of Powder Technology Japan. All rights reserved.