Single crystal titanium nitride powder was used to fabricate titanium nitride films using a vacuum kinetic spray (VKS) process. Field emission scanning electron microscopy (FESEM) and transmission electron microscopy (FETEM) were used to investigate the microstructure of the as‐fabricated films under different process conditions. Plastic deformation features (i.e., amorphization, rotated grain, slip bands, and distorted lattices in the transition structure) revealed an elastic‐to‐inelastic transition of titanium nitride particles at high strain rate and high pressure induced by hypervelocity impact, which was considered vital for grain refinement and film growth during the process.