TiAlN, and TiAlN/CrN nanolayered coatings were synthesized by cathodic-arc evaporation with plasma enhanced duct equipment. Chromium and TiAl (50/50 at %) alloy cathodes were used for the deposition of TiAlN/CrN coatings. The effects of bilayer thickness and chromium content on the microstructure and mechanical properties of TiAlN/CrN nanolayered coatings were studied. The preferred orientation was changed from (200) in TiAlN monolayered coatings to (111) plane in the multilayered TiAlN/CrN coatings. The multilayered TiAlN/CrN coating with periodic thickness of 20 nm and the smallest crystallite size of 28 nm exhibited the highest hardness of 39 GPa. The multilayered TiAlN/CrN coatings also showed the best adhesion strength using scratch tests. It has been found that the structural and mechanical properties of the films were correlated with the addition of chromium and nanolayer thickness.