This work explores the pivotal role of laser lift-off (LLO) as a vital production process in facilitating the integration of Micro-LEDs into display modules. We specifically investigate the LLO process applied to high-performance gallium nitride (GaN)-based green Micro-LED arrays, featuring a pixel size of 20 × 38 μm on a patterned sapphire substrate (PSS). Scanning electron microscopy (SEM) observations demonstrate the preservation of the GaN film and sapphire substrate, with no discernible damage. We conduct a comprehensive analysis of the optoelectrical properties of the Micro-LEDs both before and after the LLO process, revealing significant enhancements in light output power (LOP) and external quantum efficiency (EQE). These improvements are attributed to more effective light extraction from the remaining patterns on the GaN backside surface. Furthermore, we examine the electroluminescence spectra of the Micro-LEDs under varying current conditions, revealing a slight change in peak wavelength and an approximate 10% decrease in the full width at half maximum (FWHM), indicating improved color purity. The current–voltage (I–V) curves obtained demonstrate the unchanged forward voltage at 2.17 V after the LLO process. Our findings emphasize the efficacy of LLO in optimizing the performance and color quality of Micro-LEDs, showcasing their potential for seamless integration into advanced display technologies.