Ti–Si–C–N thin films with composition of 1–11at.% Si and 1–20at.% C have been deposited onto cemented carbide substrates by arcing Ti–Si cathodes in a CH4+N2 gas mixture and, alternatively, through arcing Ti–Si–C cathodes in N2. Films of comparable compositions from the two types of cathodes have similar structure and properties. Hence, C can be supplied as either plasma ions generated from the cathode or atoms from the gas phase with small influence on the structural evolution. Over the compositional range obtained, the films were dense and cubic-phase nanocrystalline, as characterized by X-ray diffraction, ion beam analysis, and scanning and transmission electron microscopy. The films have high hardness (30–40GPa by nanoindentation) due to hardening from low-angle grain boundaries on the nanometer scale and lattice defects such as growth-induced vacancies and alloying element interstitials.