The effect of Fe content on FeMn/MgO catalysts for light alkenes synthesis through CO hydrogenation was investigated. Catalysts were prepared by a conventional co-impregnation method, characterized using BET, X-ray powder diffraction (XRD) and Temperature-programmed reduction (H2-TPR) techniques. High activity was obtained over the catalyst with 9 wt-% Fe content, over which CO conversion and the selectivity of C2−-C4− reached 91.36% and 58.48%, respectively. With the increase of Fe content, both the conversion and the selectivity were improved within a certain range and then decreased. The results show that the surface area of the catalyst played an important role in the catalytic reaction. With the increase of Fe loading, the interaction action between Fe and Mn was enhanced and FeMn solid solution was formed.