The variation of the ratio between metal elements in nitride hard films is one of the important research directions for regulating the comprehensive mechanical properties of hard films. In this study, TiAlZrN hard films with fixed Al content (35-37 at%) and different Zr/Ti molar ratios were prepared by designing combinations of single Zr targets, TiZr and TiAl alloy targets, and by adjusting the target current. The crystal growth, phase structure, and hardness of TiAlZrN hard films with different Zr/Ti molar ratios and friction and wear properties were investigated. The experimental results show that the droplets on the surface of TiAlZrN hard films prepared using Zr-containing targets increased significantly. The hard film exhibits TiAlZrN (111) crystal face-oriented growth on a selective basis. The TiAlZrN hard film with a Zr/Ti molar ratio of 0.49 has the highest hardness value of 45.1 ± 1.5 GPa. TiAlZrN hard films with a Zr/Ti molar ratio of 0.80 have the best wear resistance with a friction coefficient of 0.4–0.6 and a hardness value of 39.2 ± 1.5 GPa. Higher hardness values lead to more severe abrasive wear and influence the wear resistance of hard films. This study provides a reliable basis for the design of hard film compositions with excellent overall mechanical properties.