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The glass fiber-reinforced polypropylene/AA2024 hybrid composite (short for Al/Gf/PP laminate) was prepared by hot pressing with anodized 2024-T3 aluminum alloy as the skin and thermoplastic glass fiber-reinforced polypropylene core as a substitute of thermosetting glass fiber-reinforced polymer (based on epoxy) in order to increase the productivity and reduce the production costs during manufacturing procedure. The effect of peel ply (release cloth) and cooling rate on the laminate was investigated elaborately in this work. The orientation of glass fiber is mainly influenced by the peel ply structure, resulting in the resin’s overflow during hot press. Moreover, different cooling rates due to various cooling methods significantly affected both the degree of crystallization of the matrix and deformation of the metal skin during the curing process. Finally, a new peel ply structure was adopted to prevent the fiber from spilling during hot press process, while bubbles were allowed to flow out normally along with partial resin. Finally, a novel cooling method to reduce the degree of polypropylene crystallization and control metal deformation was proposed.