Graphene nanoplatelets (GNPs) reinforced 7075 aluminum (Al) nanocomposites were successfully synthesized using the powder metallurgy method. A novel method for optimizing interfacial bonding by coating titanium dioxide (TiO 2 ) on the surface of GNPs was proposed in this manuscript. The effects of GNPs on mechanical properties and microstructure of the aluminum matrix nanocomposites, both with and without TiO 2 coating layers, have been investigated. Experimental results showed that the corresponding mechanical properties of the nanocomposites were further improved when the GNPs have TiO 2 coating layers, compared with the addition of pure GNPs. The yield strength, ultimate tensile strength, and microhardness of the nanocomposites reinforced with TiO 2 -coated GNPs increased by 22.9%, 25.9%, and 20.1%, respectively, in comparison to those of the matrix. The further improvement of the mechanical properties could be attributed to the existence of the coating layer, which optimizes the interface bonding between the reinforcement and the matrix, thereby improving the effectiveness of load transfer.