This study investigates the influence of varying Al/Cr ratios on the material properties of (Al 30– 40Cr 30– 20Nb 15Si 10Ti 15)N high-entropy nitride coatings. Grazing incidence X-ray diffraction (GIXRD) and selected area electron diffraction (SAED) analyses reveal a clear texture shift from (111) to (200)/(220) orientations and significant grain refinement with increasing Al content, attributed to the formation of strong Al–N bonds and elevated residual stress. Tribological testing shows a reduction in the coefficient of friction (COF) from 0.71 to 0.55 and narrower wear tracks at higher Al/Cr ratios, indicating improved wear resistance. Nanoindentation results demonstrate enhanced hardness (from 26.9 to 31.7 GPa) and elastic modulus (from 311.3 to 326.5 GPa). However, increased Al content also promotes brittle behavior, with lateral cracking and pop-ins, marking a shift toward a brittle-dominant deformation mechanism.