Nano-crystalline diamond (NCD) films with good adhesion were deposited on flexible copper substrate with Ni interlayer by Microwave Plasma Chemical Vapor Deposition (MPCVD). In this paper, two-stage method was used to improve the adhesion between the copper substrates and the diamond films. The effect of deposition time of the first stage on the morphology, crystal structure, non-diamond phase and adhesive properties of diamond films was investigated. The performance and structure of the diamond films were studied by Scanning Electron Microscope (SEM), Raman Spectroscopy (Raman) and X-Ray Diffraction (XRD). The results showed that the films were nano-crystalline diamond films positively. Impress method was used to examine the adhesion between diamond film and the substrate. When deposition time is 1.5h, the adhesion between diamond film and the copper substrate is better than the others. When it was 2.5h or longer, because the graphite layers existed as intermediate, the adherence between the diamond films and copper substrates was very poor. Therefore, the diamond films were easily peeled off from the substrates. Otherwise, the second stage called annealing process after the deposition played an important role to the adhesion. The films would be easily peeled off by curling without the annealing process.