WC-10Co-4Cr coating is highly valued for its corrosion resistance and wear resistance when applied using the high-velocity oxy-fuel (HVOF) spraying method. However, conventional grinding (CG) of this coating presents challenges, including substantial grinding forces and elevated surface temperatures. To address these concerns, our study proposed the utilization of ultrasonic vibration-assisted grinding (UVAG) as a means to enhance the machining properties of HVOF-sprayed WC-10Co-4Cr coatings. Comparative experiments were conducted to analyze the impacts of various factors on the grinding forces and surface roughness in UVAG and CG processes. Additionally, the topography of the ground surfaces was examined to gain insights into the material removal mechanism in UVAG. The experimental outcomes reveal significant reductions in tangential and normal grinding forces, amounting to 15.47% and 22.23%, respectively, in UVAG when compared with CG. Furthermore, UVAG led to a roughly 29.14% decrease in ground surface roughness compared with CG. Microscopic analysis of the ground surfaces using scanning electron microscopy (SEM) indicated that ductile removal was the predominant material removal mode in UVAG. Overall, UVAG was found to be effective in diminishing grinding forces, improving ground surface roughness, and enhancing surface integrity when contrasted with CG. These findings introduce a novel approach for processing WC-10Co-4Cr coatings.