Despite its unrivaled hardness, polycrystalline diamond can be severely worn under the interaction with softer copper during the ultrafine copper wire drawing process. The influence of the polycrystalline diamond surface state on its friction behavior is investigated in this work, and argon, oxygen, and hydrogen plasma treatments are adopted to regulate the surface state of diamond. When sliding against copper, the original diamond plate exhibits a coefficient of friction (COF) exceeding 0.4, copper wears by transferring to the diamond, and diamond wears owing to the carbon cluster removal, as confirmed by the TOF-SIMS analyses of the obvious wear tracks. After hydrogen plasma treatment, the tribological performance of diamond sliding against copper is most significantly improved, in which the COF is more stable and reaches 0.18 with minimal wear debris. Hydrogen plasma treatment generates more hydrogen termination on the diamond surface as well as a hydrogen-containing amorphous carbon layer, which provides an isolated lubrication effect and strongly reduces adhesive wear. Argon plasma treatment also decreases the level of COF to a certain extent, which is attributed to its polishing and cleaning action that removes surface contamination and reduces roughness. In contrast, oxygen plasma treatment induces a pronounced etching effect, resulting in groove-like protrusions on the diamond surface that exacerbates abrasive wear. Our research provides a more sustainable and residue-free solution for minimizing friction and wear of polycrystalline diamond wire drawing dies.