Design of hard ceramic material coatings with enhanced toughness, which prevents crack formation/propagation leading to brittle failure during application, is a primary industrial requirement. In this work, experimental methods supported by ab initio density functional theory (DFT) calculations and electronic structure analyses are used to investigate the mechanical behavior of magnetron sputtered Ti-Al-Ta-N hard coatings. The as-deposited Ti1-x-yAlxTayN (y = 0-0.60) films exhibit a single phase cubic sodium chloride (B1) structure identified as TiAl(Ta)N solid solutions. While the hardness H of Ti0.46Al0.54N (32.5 +/- 2 GPa) is not significantly affected by alloying with TaN (H of the quaternary nitrides varies between 26 +/- 2 and 35 +/- 4 GPa), the elastic stiffness monotonically decreases from 442 to 354 GPa with increasing Ta contents, which indicates improved toughness in TiAlTaN. Consistent with the experimental findings, the DFT results show that Ta substitutions in TiAlN reduce the shear resistance due to the enhanced occupation of metal-metal bonding states while preserving strong metal-N bonds. The metal-N bonding character, however, is progressively modified from prevalently ionic (TiAlN) toward more covalent (TiAlTaN). (C) 2017 American Vacuum Society.