By designing different interlayers (Al, Si/SixNy and Cr interlayer) and oxygen plasma pretreatment of the substrate, strong adhesion was realized for the double-layer flexible copper clad laminate on polyimide (PI) substrate via high power impulse magnetron sputtering (HiPIMS) technology. The microstructures and properties of Cu films on PI substrate were characterized by an X-ray powder diffractometer (XRD), X-ray photoelectron spectroscope (XPS), atom force microscopy (AFM), scanning electron microscope (SEM), nano-scratch test, scotch tape test and four-probe detector. With the introduction of interlayer and oxygen plasma pretreatment, the critical load of Cu film (300 nm thick) peaked at 43.5 mN and the sheet resistance ranged from 124 to 227 mΩ/sq. The oxygen plasma pretreatment resulted in the drastic oxidation to generate functional groups on the PI substrate surface, which contributed to the improvement of adhesion strength by chemical interaction in terms of the film with Si/SixNy or Cr interlayer. Besides, for the Cu film with Si/SixNy interlayer, the resistance against copper diffusion by the SixNy layer can also promote the enhancement of adhesion strength.