Ti-containing amorphous carbon (Ti-aC) coatings were deposited on cemented carbide and Si substrates by cathode-arc-enhanced closed field middle-frequency unbalanced magnetron sputtering. The coatings were studied by using atomic force microscopy, Raman scattering, nanoindentation, and pin-on-disk testing. The measurements showed that the hardness of the coatings increased from 12 GPa at a Ti content of 1 at.% to 27 GPa at 31 at.%. The coatings exhibited different friction behaviors when facing different mating materials and changed with increasing Ti content. The coating with 4 at.% Ti exhibited excellent tribological performance with a low friction coefficient of 0.07when facing the cemented carbide.