Compounding Au-Ni with carbon (C) lubricants is a feasible approach to improve its mechanical properties and wear performance. In this study, 3.5 µm-thick Au-Ni/C nanocomposite coatings with a low residual stress on CuCrZr substrates by magnetron sputtering were developed. Face-centered cubic and hexagonal close-packed stacking structures were both confirmed in the composite coatings based on transmission electron microscopy and X-ray diffraction analyses. Amorphous C (a-C) was confirmed to be the structure of C in the composite coatings, and its graphitization transition with an increase in the C content was validated by X-ray photoemission spectra and Raman spectroscopy. By compounding 0.88 wt.% a-C, the hardness of the Au-Ni/a-C coating reached 400 HV, which is twice higher than that of the Au-Ni coating. The electrical resistivity of the Au-Ni/a-C coating is relatively stable with an increase in the a-C content. As graphitization occurred on the wear track, the produced composite coatings showed a minimum wear rate of 2.2×10-6 mm 3 /N·m under atmospheric conditions, which is half that of the Au-Ni reference coating. Under vacuum, the wear performance of the produced Au-Ni/a-C composite coatings was similar to that of the Au-Ni reference coating.