Two series of non-hydrogenated diamond-like carbon (DLC) films and molybdenum doped diamond-like carbon (Mo-DLC) films were grown on the silicon substrate using direct current magnetron sputtering. The influence of molybdenum doping (between 6.3 and 11.9 at.% of Mo), as well as the deposited temperature (between 185 and 235 °C) on the surface morphology, elemental composition, bonding microstructure, friction force, and nanohardness of the films, were characterized by atomic force microscopy (AFM), energy dispersive X-ray spectroscopy (EDX), Raman spectroscopy, and a nanoindenter. It was found that the increase in the metal dopant concentration led to a higher metallicity and graphitization of the DLC films. The surface roughness and sp3/sp2 ratio were obtained as a function of the Mo concentration and formation temperature. The nanohardness of DLC films was improved by up to 75% with the addition of Mo. Meanwhile, the reduction in the deposition temperature decreased the nanohardness of the DLC films. The friction coefficient of the DLC films was slightly reduced with addition of the molybdenum.