Abstract Reliable metallization of polymer substrates is essential for flexible electronics, advanced packaging, and high-frequency systems, yet achieving strong metal/polymer adhesion while maintaining good electrical performance remains challenging. Here, carbon-ion, nitrogen-ion, and carbon/nitrogen dual-ion implantation were used to modify polyimide, with the implantation conditions independently adjusted to obtain nearly identical surface free energies of 46.43–47.22 mJ m-2.