This study focuses on modifying the surface of an AA 5052-H32 aluminum alloy using plasma treatment. Discharge power, exposure time, and working gas were adjusted as process parameters to improve the adhesion between the aluminum alloy and glass fiber-reinforced thermoplastic (GFRTP) polycarbonate composite. The surface composition and morphology of the aluminum alloy sheet were analyzed by X-ray photoelectron spectroscopy and scanning electron microscopy, and surface roughness and wettability were evaluated using a surface roughness-measuring instrument and contact angle goniometry, respectively. The bonding performance of GFRTP/aluminum alloy was also assessed. The surface of the aluminum alloy was subjected to chemical treatment prior to plasma treatment. The results revealed that nitrogen plasma treatment led to a substantial increase (25%) in bonding strength due to the synergistic effect of rough surface mechanical bonding and chemical bonding through functional groups between the aluminum alloy and GFRTP. However, the improvement in surface wettability by plasma treatment is time dependent and may gradually diminish over time due to the re-adsorption of hydrocarbon contamination from the surrounding air.