Diamond-like carbon (DLC) bilayer films with Cu interlayer were prepared on silicon substrate by direct-current and pulsed cathode arc plasma technique, and annealed at various temperatures in vacuum. Structure, morphology and mechanical properties of the bilayer films were investigated by Raman spectroscopy, Auger electron spectroscopy, scanning electron microscopy and atomic force microscopy, surface profilometer and Vickers sclerometer. The results show that Cu interlayer changes the bilayer microstructure, including the thickness and element distribution of diffusion layer, the relative fraction of sp3/sp2bonding and growth model of bilayer. A simple three-layer model was used to describe the interdiffusion between Cu and C layer. Cu interlayer could be more effective against graphitization upon annealing. Morphological characteristics of the films were studied by analyzing the surface features of substrate. Cu/DLC bilayer exhibits highly dispersed nano-agglomerates with smaller size on the surface due to low surface energy of Cu interlayer. The stress and hardness of the films were affected accordingly. Cu/DLC bilayer shows a relatively high hardness at low annealing temperature but the stress almost no change. By changing Cu interlayer and annealing temperature, excellent DLC films could be designed for the protective, hard, lubricating and wear resistant coatings on mechanical, electronic and optical applications.