This study systematically studied the effect of gradient variation of Si-content on the microstructure evolution and wear performance of multilayer Fe-based ultrafine-grained coatings. When the Si-content ranged from 1.5 to 2.5   wt.%, Si-related diffraction peaks emerged in the top layer of the coating. As Si-content increased, both grain size and carbide size of the coating initially decreased and then increased. When the Si-content was 2.0   wt.%, the grain and carbide size reached the minimum values of 0.86 μm and 1.04 μm, respectively. Correspondingly, the microhardness of the coating showed a trend of initially increasing and then decreasing, peaking at an average value of 1144 HV 0.2 in the top layer at 2.0   wt.% Si. At room temperature and 400 °C, the wear resistance of the coating followed a similar trend, improving initially with increasing Si-content and then declining. Optimal wear resistance was achieved at 2.0   wt.% Si, with wear rates of 0.264×10 −6 mm 3/(N·m) at room temperature and 3.37×10 -6 mm 3/(N·m) at 400 °C.