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.