In this work, we put forward a rigorous study on ultraviolet (355-nm) laser irradiation of polyimide for the realization of high-quality laser-induced graphene (LIG) with micron-scale features. High-quality material and micron-scale features are desirable—but often at odds—given that small features demand tightly focused beam spots, with a predisposition to ablation. As such, we investigate the synthesis of LIG by correlating the material characteristics, as gleaned from scanning electron microscopy and Raman spectroscopy, to the incident optical fluence, as a measure of applied optical energy per unit area. The study reveals that high-quality LIG, with ratios of Raman 2D-to-G peak heights approaching 0.7, can be synthesized with micron-scale features, down to 18 ± 2 μm, given suitable attention to the optical fluence. Optimal characteristics are seen at optical fluences between 40 and 50 J/cm2, which promote graphenization and minimize ablation. It is hoped that these findings will lay a foundation for the application of LIG in future integrated technologies.