Abstract Chromium copper–diamond-like carbon (Cr:Cu)-DLC films were deposited onto silicon and by cathodic arc evaporation process using chromium (Cr) and copper (Cu) target arc sources to provide Cr and Cu in the Me-DLC. Acetylene reactive gases were the carbon source and activated at 180 °C at 13 mTorr, and a substrate bias voltage was varied from −50 V to −200 V to provide the (Cr:Cu)-DLC structure. The structure, interface, and chemical bonding state of the produced film were analyzed by transmission electron microscope (TEM), IR Fourier transform (FTIR) spectra, and X-ray photoelectron spectroscopy (XPS). The results showed that the Cr-containing a-C:H/Cu coatings exhibited an amorphous layer of DLC:Cr layer and a crystalline layer of Cu multilayer structure. The profiles of sp 3 /sp 2 (XPS) ratios corresponded to the change of microhardness profile by varying the pressure of the negative DC bias voltage. These (Cr:Cu)-DLC coatings are promising materials for soft substrate protective coatings.