The present work describes the hybrid layers consisting of 1-μm-thick hydrogenated diamond-like carbon (DLCH) film deposited by ion beam deposition (IBD) method as the bottom layer and spin coating polyimide (PI) film at a thickness of 6 μm as the top layer. Optical microscopy shows that all DLCH film, PI film and PI/DLCH film have smooth surface and are free from cracks or wrinkles. Water contact angle measurement shows that the annealed DLCH film has the higher relative adhesive tension and adhesive work than that of PI film. Raman spectra show that the DLCH film can avoid severe graphitization & degradation at 300°C during annealing treatment, and FTIR spectra also exhibit that the PI film will reach 95% imidization during the curing step at 300°C. PI film can act on DLCH film as the stress buffer. This is demonstrate from warpage measurement showing that top PI film with tensile stress can partially reduce the compressive stress over bottom DLCH film with 6.7% warpage reduction. The electrical resistivity of PI/DLCH/Si is similar to that of PI/Si is resulted from the PI passivation effect.