In tribological applications, the degradation of alloy nitride coatings is an issue of increasing concern. The drawbacks of monolayer hard coatings can be overcome using a multilayer coating system. In this study, single-layer TiAlNbN and multilayer TiAlNbN/AlCrN coatings with AlCrN layer addition into TiAlNbN were prepared by cathodic arc evaporation (CAE). The multilayer TiAlNbN/AlCrN showed B1 NaCl structure, and the columnar structure continued from the bottom interlayer of CrN to the top multilayers without interruption. After AlCrN addition, the TiAlNbN/AlCrN coating consisted of TiAlNbN and AlCrN multilayers with a periodic thickness of 13.2 nm. The layer thicknesses of the TiAlNbN and AlCrN were 7 nm and 6.2 nm, respectively. The template growth of the TiAlNbN and AlCrN sublayers stabilized the cubic phases. The introduction of bottom CrN and the TiAlNbN/CrN transition layers possessed com-position-gradient that improved the adhesion strength of the coatings. The hardness of the deposited TiAlNbN was 30.2 ± 1.3 GPa. The TiAlNbN/AlCrN had higher hardness of 31.7 ± 3.5 GPa and improved tribological performance (wear rate = 8.2 ± 0.6 × 10−7 mm3/Nm) than those of TiAlNbN, which were because the multilayer architecture with AlCrN addition effectively resisted abrasion wear.