The cutting properties of tools can be greatly improved by AlCrSiN coatings. The AlCrSiN coatings with nitrogen content in the range of 28.2–56.3 at.% were prepared by varying the N2/Ar flow ratio from 1/4 to 1/1. The influence of N2/Ar flow ratio on composition, microstructure, and mechanical properties, as well as the tribological properties, of the coatings was investigated. With increasing N content, the coating microstructure gradually evolved from single fcc-(Cr,Al)N (200) phase to the mixture of fcc-(Cr,Al)N and hcp-(Cr,Al)N phase, which corresponds to an increased crystallinity within the coatings. The coating presents the highest hardness and best wear resistance for an N2/Ar flow ratio of 1/1, but the film adhesive strength and inner stress decreased obviously with increasing N2/Ar flow ratio, which was attributed to the rapid reduction of particle kinetic energy induced by the obstruction of neutral nitride particles between target and substrates. The highest H3/E*2 value exhibited the lowest wear rate, at 0.81 × 10−14 m3/(N·m), indicating that it had the best resistance to plastic deformation. The main wear mechanisms of the as-deposited coatings were abrasive wear and adhesive wear. The increasing crystallinity of the interior coatings resulted in higher hardness and better tribological behavior with an increase in N2/Ar flow ratio.