The HfZrC coatings containing varying carbon contents were fabricated by magnetron sputtering method. The relationship between coating composition and mechanical properties as well as tribological behavior was studied. The coatings containing lower carbon are mainly composed of (Hf,Zr)C carbide, less metal and amorphous graphite-like carbon (GLC). The increasing carbon contents significantly favored the formation of (Hf,Zr)C carbide, leading to the enhanced hardness and elastic modulus. Excessive carbon increased the GLC content, thus degrading the two aforementioned performances. During the friction process, the low-carbon coating fractured in a short friction duration due to the remarkable shear stress. The abrasive wear dominated the following friction process, resulting in severe wear loss of TC4 substrate. Comparatively, the lubricant GLC in high-carbon coating alleviated the coating fracture. Hence, the wear rate of high-carbon coatings was decreased significantly by inhibiting the abrasive wear.