This study investigates the deposition of CrAlYN nanomultilayer films with different yttrium (Y) contents on M2 tool steel and single-crystal Si wafer using unbalanced magnetron-sputtering ion-plating technology. Transmission and scanning electron microscopic and scanning morphologies, X-ray diffraction pattern, energy dispersive spectra, nanoindentation, high-temperature oxidation, and high-temperature tribological analyses show that CrAlYN nanomultilayer films have a face-centered cubic (fcc) crystal structure with a modulation period of CrN/YN+AlN/CrN/AlN. CrAlYN films exhibit optimal mechanical performance when Y content is 1.13at%. However, a substantial drop occurs when Y content increases to 2.67at%. As Y content increases, the high-temperature oxidation resistance, friction, and wear of CrAlYN films first increase and then decrease. Notably, films with the Y content of 1.13at% have optimal resistance to high-temperature oxidation, friction, and wear.