Polyimide (PI) films are widely used in electronic devices owing to their excellent mechanical and electrical properties and high thermal and chemical stabilities. In particular, PI films play an important role in flexible printed circuit boards (FPCBs). However, one challenge currently faced with their use is that the adhesives used in FPCBs cause a high dielectric loss in high-frequency applications. Therefore, it is envisioned that PI films with a low dielectric loss and Cu films can be used to prepare two-layer flexible copper-clad laminates (FCCLs) without any adhesive. However, the preparation of ultra-thin FCCLs with no adhesives is difficult owing to the low peel strength between PI films and Cu films. To address this technical challenge, an FCCL with no adhesive was prepared via high-power helicon wave plasma (HWP) treatment. Field-emission scanning electron microscopy (FE-SEM), X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD) were tested. Also, the surface roughness of the PI film and the peel strength between the PI film and Cu film were measured. The experimental results show that the surface roughness of the PI film increased by 40–65% and the PI film demonstrated improved adhesion (the peel strength was >8.0 N/cm) with the Cu film following plasma treatment and Cu plating.