Laser cleaning is an advanced surface pretreatment technology, which can remove pollutants on the surface of composite materials, such as release agent, with minimal damage to the reinforcement phase in the composite materials. Due to the strong light transmission of the release agent, the laser directly irradiated on the release agent is easy to damage the glass fiber. In this paper, the orthogonal experiment method is used to remove the release agent layer with black paint coating on the surface of glass fiber reinforced resin matrix composite (GFRP) by using infrared pulse laser. The purpose is to effectively remove the release agent on the surface of GFRP, ensure that the damage to glass fiber is minimized and improve the surface roughness. Cutting glass fiber resin matrix composites into 25 mm×15 mm×2 mm rectangular test piece quickly and efficiently using advanced water guided laser machine tools, wiped with absolute ethanol and dried in the air. Before the cleaning test, evenly spray a layer of about 100 μm thick on the surface of the test piece black paint layer and natural drying for 5 min. In the test, a 50 W infrared pulse laser with a focal length of 160 mm and a laser spot diameter of 0.85 mm was used. The laser parameters used are average power (15, 20, 25 and 30 W), laser scanning speed (240, 250, 255 and 260 mm/s) and laser pulse frequency (70, 80, 90 and 100 kHz). Then, the surface morphology of the cleaning layer of each specimen was observed by Caikang microscope (XTL-3400C) and the microstructure of the cleaning layer of each specimen was observed by scanning electron microscope (Zeiss EVO10). Use a white light interferometer (ContourGT-X) to detect the surface roughness values at three positions on the cleaning layer surface of each test piece and calculate the average value as the final surface roughness value. When the laser parameters are average power P=25 W, laser scanning speed v=255 mm/s, and laser pulse frequency f= 100 kHz, the release agent can be effectively removed, and the integrity of the glass fiber is retained, and the surface roughness Sa changes from the original 0.684 μm increases to a stable value of (4.5±0.3) μm. With the increase of the average power, the surface roughness Sa of the specimen increases gradually, its bonding strength is higher than that without surface treatment; With the increase of scanning speed, the surface roughness Sa of the specimen decreases first and then increases; With the increase of pulse frequency, the surface roughness Sa of the specimen decreases gradually. The optimal experimental preparation laser cleaning process parameters are average power P=25 W, laser scanning speed v=255 mm/s, and laser pulse frequency f=100 kHz. Under these parameters, the mold release agent can be effectively removed, the damage of glass fiber can be minimized, and the surface roughness can be improved to effectively and ensure the surface quality of GFRP sheets. At the same time, it is also conducive to improving the bonding strength between composite materials. The research results can provide a reference for laser cleaning of composite mold release agent in the aviation field.