An inkjet-based ultrashort pulsed laser patterning on a polymer substrate is presented with high-laser scanning speeds. The effects of the laser processing parameters on the ablation characteristics were studied to accomplish damage-free laser ablation. Laser ablation characteristics depend on input energy, scanning speed, and number of scans. Final width of microelectrodes can be flexibly controlled by multiple selective ablations. Well-defined, uniform microelectrodes without damaging their microstructure, and the underlying polymer substrate are demonstrated via a direct pattering process combining inkjet printing with ultrashort pulsed laser ablation. These microelectrodes exhibit little influence of thermal effect of laser ablation, resulting in little variation in their electrical performances.