We studied on a nanometer scale the tribological properties of thin silicon carbide films on Si(100) wafers and stainless steel. The coatings were fabricated from a sintered SiC target by pulsed ArF laser deposition at substrate temperatures between 20 °C and 1000 °C. Amorphous films resulted at low deposition temperatures while nanocrystalline structures developed at high deposition temperatures. An atomic force/lateral force microscope was employed to characterize the film topography and the friction behavior. The microhardness was determined from measurements utilizing a depth-sensing nanoindentation instrument. The SiC films on Si(100) exhibit a smooth surface with an average roughness Ra of a few nanometer, the amorphous films being even an order of magnitude smoother. No appreciable differences were found in microhardness and friction coefficient between amorphous and nanocrystalline films. On stainless steel, amorphous SiC coatings were obtained for deposition temperatures up to 500 °C. Their surface relief portrayed the grain boundaries of the underlying steel substrate, reflecting the ballistic nature of the deposition process. No stoichiometric films were obtained above 500 °C as the silicon from the growing film quickly dissolved in the steel substrate.