ZnO nanoparticles-embedded hydrogenated diamond-like carbon (ZnO-DLC) films have been prepared by electrochemical deposition in ambient conditions. The morphology, composition, and microstructure of the films have been investigated. The results show that the resultant films are hydrogenated diamond-like carbon films embedded with ZnO nanoparticles in wurtzite structure, and the content and size of the ZnO nanoparticles increase with increasing deposition voltage, which are confirmed by X-ray photoelectron spectroscopy (XPS), Raman, and transmission electron microscope (TEM). Furthermore, a possible mechanism used to describe the growth process of ZnO-DLC films by electrochemical deposition is also discussed.