A series of FeCrBCSi coatings were prepared by two-roll wire-arc spraying to investigate the influence of the boron content on the microstructure and properties of the coatings. Microstructural studies show that the as-deposited coatings present a dense layered structure with the porosity around 3%, and are primarily composed of a composite structure of amorphous phase and nanocrystalline phase. It is found that the addition of boron content within the composition range examined exhibits a significant effect on the phase component, as well as the microhardness and wear resistance of the coatings. The optimal composite phase structure, in terms of higher amorphous fraction and lesser nanocrystalline size distribution, leads to the relatively best performance of the coating with 26% boron added. The relative wear resistance of this coating is about 18 and 4 times higher than that of the Q235 steel and commercially available SHS 7170 coating, respectively, therefore wire-arc sprayed FeCrBCSi coating could be an effective and economic approach to withstand wear environment.