Currently, seldom studies have paid close attention to the impact of the defects and oxygen-containing functional groups on the surface of the graphene for composite applications. In this work, two typical graphene materials, namely graphene nanosheets synthesized by an in situ catalytic reaction and reduced graphene oxide (RGO), were adopted to fabricate reinforced copper matrix composites by spark plasma sintering. A harmful transitional interfacial layer made up of Cu/CuOx/amorphous carbon/RGO, resulted from interfacial reaction between Cu and RGO, were observed in the RGO/Cu composite. In contrast, the in situ synthesized graphene with fewer defect and lower oxygen level can realize clean graphene-Cu interface with Cu-O-C bonding and thus lead to much improved interface bonding and superior yield strength and tensile ductility. These results imply that the in situ synthesized graphene is more favorable for achievement of robust interfacial bonding for enhancing the mechanical properties of the graphene-Cu composites.