A titanium carbide (TiC) nanostructured coating and Ti intermediate layer are fabricated on NiTi by plasma immersion ion implantation and deposition (PIII&D) to improve the surface properties. The chemical composition and structure are determined by X-ray diffraction, Auger electron spectroscopy, scanning electron microscopy, and atomic force microscopy. Nano-indentation is used to evaluate the mechanical properties of the thin film and the biological characteristics are assessed by electrochemical measurement and soaking tests in simulated body fluids. Based on the potentiodynamic polarization and Ni release data after the polarization test, the Ti/TiC nanostructure coating has better corrosion resistance compared to the NiTi substrate and there is significantly less Ni ion release from the NiTi substrate into the simulated body fluids than the uncoated NiTi alloy.