Nanocarbon materials, such as graphene, carbon nanotubes, and their derivatives, are considered highly effective reinforcing agents in metals. Copious experimental and computational observations suggest that the nature of the interfaces may significantly affect the mechanical behavior of nanocarbon-metal composites, while the exact correlation between the interfacial structure and the deformation and failure mechanisms of the composite remains elusive. Using a nanolaminated graphene-aluminum (Al) composite as the model material, we designed and created composites with distinct interfacial structures and bonding states via graphene functionalization. The mechanical behavior of the composites was strongly affected by the structure of the functionalized graphene (FG)/Al interface, and the optimum strength-ductility synergy came from the composite with the intermediate extent of functionalization. Complementing experimental results with molecular dynamics and phase-field simulation efforts, we interpreted these results by the combined effects of the intrinsic strength of FG nanosheets and the FG/Al interfacial bonding state.