A physical vapor deposition process using anodic arc evaporation in combination with a hollow cathode arc discharge was applied to the evaporation of graphite for deposition of hydrogen-free carbon layers. The diamond-like carbon (DLC) films deposited on 100Cr6 steel substrates were investigated by nanoindentation, Raman spectrometry, FE-SEM, AFM and spectroscopic ellipsometry. The relationships between the process parameters and the coating properties are discussed. Coatings deposited without bias voltage at substrate temperatures <200 °C are very hard (61–75 GPa) with also very high Young's modulus (588–685 GPa). The evaluation of the Raman spectra indicated a high proportion of tetrahedral sp3 bonds in the range of 70–88 %. Obviously, the vapor particle energies are high enough to achieve such high hardness values even without application of a bias voltage. The coatings proved to be completely droplet-free and have a very low surface roughness as confirmed by FE-SEM and AFM. The deposition rates in the range of 4–18 nm/s are exceptionally high for such tetrahedral amorphous carbon (ta-C) coatings, which is a good prerequisite for industrial applications. The ta-C layers with very high hardness and smooth surface are well suited as wear resistant layers.