Al2O3-reinforced Fe901 metal-ceramic composite coatings were prepared by laser cladding to improve the wear resistance of surface coating of metal materials. This study investigated the effect of Al2O3-reinforced phase on the microstructure and properties of a Fe-based cladding layer. The microstructural evolution, phase compositions, wear resistance, and microhardness of the composite coatings were studied using scanning electron microscopy, X-ray diffraction, friction and wear tester, as well as microhardness tester, respectively. The results show that the microstructure of the Fe901 coating was dominated by columnar and equiaxed dendrites. In addition, the addition of Al2O3 promoted the transformation of microstructure into a uniformly distributed white network-like intergranular structure with wrapped fine black grains. The surface of Al2O3 ceramic particles micro-melted and combined with Fe and Cr to form Fe3Al and (Al, Fe)4Cr intermetallic compounds within the composite coating, which increased the bond strength between Al2O3 ceramic particles and the metal phase. When the mass fraction of Al2O3 ceramic particles is 10%, the microhardness of the composite coating is increased by 16.4%, and the mass loss in the composite coating is reduced by 50% compared to that of the Fe901 coating. Thus, adding an adequate amount of Al2O3 ceramics can improve the microhardness and wear resistance of coatings.