Diamond-like carbon (DLC) films were successfully deposited on micro-textured copper substrates via aqueous electrodeposition at 60 °C. The influence of picosecond laser surface texturing (ps-laser surface texturing) parameters on micro-textured morphology and the growth mechanism of the films were systematically investigated. The microstructure, hydrophobicity, corrosion resistance, and wear resistance of the films were analyzed at different voltages (4.0–8.0 V). The results demonstrate that the micro-textured surface-assisted electrodeposition achieved optimal performance at 7 V. Raman and XPS analyses revealed that the films deposited under optimal conditions exhibited the lowest I D /I G ratio and higher sp 3-C content, indicating a more diamond-like carbon structure. FTIR analysis confirmed the prepared films as hydrogenated amorphous carbon (a-C: H). Under micro-texture assistance at 7 V, the films deposition rate reached approximately 3 μm·h −1 in formic acid aqueous solution, while demonstrating improved corrosion resistance and wear performance.