Due to their applicability for manufacturing dense, hard and stable coatings, Physical Vapor Deposition (PVD) techniques, such as High Power Impulse Magnetron Sputtering (HiPIMS), are currently used to deposit transition metal nitrides for tribological applications. Cr-Al-N is one of the most promising ceramic coating systems owing to its remarkable mechanical and tribological properties along with excellent corrosion resistance and high-temperature stability. This work explores the possibility of further improving Cr-Al-N coatings by modulation of its microstructure. Multilayer-like Cr_1−xAl_xN single films were manufactured using the angular oscillation of the substrate surface during HiPIMS. The sputtering process was accomplished using pulse frequencies ranging from 200 to 500 Hz and the resulting films were evaluated with respect to their hardness, Young’s modulus, residual stresses, deposition rate, crystallite size, crystallographic texture, coating morphology, chemical composition, and surface roughness. The multilayer-like structure, with periodicities ranging from 250 to 550 nm, were found associated with misorientation gradients and small-angle grain boundaries along the columnar grains, rather than mesoscopic chemical modulation of the microstructure. This minute modification of microstructure along with associated compressive residual stresses are concluded to explain the increased hardness ranging from 25 to 30 GPa, which is at least 20% over that expected for a film of the same chemical composition grown by a conventional PVD processing route.