The WC-10Co4Cr coatings with conventional structure and bimodal structure were sprayed by high-velocity oxygen fuel (HVOF) technology. The phase compositions and morphologies of the WC-10Co4Cr powders and coatings were analyzed by X-ray diffraction (XRD) and scanning electron microscopy (SEM). The microhardness, porosity, bonding strength, elastic modulus, and indentation fracture toughness of the conventional coating (Conventional) and the bimodal coating (Bimodal) were also studied. The sliding wear properties of the Conventional and the Bimodal against Si3N4 counterballs under different loads at room temperature (∼25 °C) were investigated using a friction and wear tester. Compared with the Conventional, the Bimodal has denser microstructure, lower porosity, more excellent mechanical properties, and the Bimodal has better wear resistance than the Conventional under different loads. The two coatings under 15 N and 30 N only exhibit abrasive and slightly adhesive wear mechanism, while in the load application of 45 N, additional mechanism which is fatigue is detected and causes flaking of the coating.