We investigated the tribological properties of amorphous carbon (a-C) films deposited with CrC interlayers of various thicknesses as the adhesive layer. A-C and CrC thin films were deposited using the unbalanced magnetron (UBM) sputtering method with graphite and chromium as the targets. CrC films as the interlayer were fabricated under a-C films, and various structural, surface, and tribological properties of a-C films deposited with various CrC interlayer thicknesses were investigated. With various CrC interlayer thicknesses under a-C films, the tribological properties of CrC/a-C films were improved; the increased film thickness exhibited a maximum high hardness of over 27.5 GPa, high elastic modulus of over 242 GPa, critical load of 31 N, residual stress of 1.85 GPa, and a smooth surface below 0.09 nm at the condition of 30-nm CrC thickness.