This work deals with the plasma surface modification of aluminum alloy AA6061-T6 by changing two key parameters of processing time and working gas to enhance the interfacial adhesion between glass fiber reinforced polypropylene layer and the aluminum alloy sheet. The surface composition and morphology of aluminum alloy sheet were characterized respectively by means of XPS and SEM with EDS, while the roughness and wettability of the surface were measured by using a surftest and a contact-angle goniometry. Moreover, the interlaminar properties and static performance of Al/Gf/PP laminates were evaluated individually. The results indicated that the laminates presented higher mechanical properties, in which the aluminum alloy sheet was modified by nitrogen plasma treatment for 10 min. This is due to the synergistic mechanism of the mechanical bonding by a rough surface and the chemical bonding by functional group (CN and CN) between the aluminum alloy sheet and glass fiber reinforced polypropylene layer. In addition, compared with the phosphoric anodic oxidation, the nitrogen plasma treatment of the aluminum alloy sheet could make the interlaminar shear properties and static performance of Al/Gf/PP laminates better.