A graphene-based composite structure is disclosed. The graphene-based composite structure includes a graphene layer, a transition metal layer, and a substrate. The graphene layer, transition metal layer, and substrate are stacked together in series to form a sandwich structure. The graphene layer and the transition metal layer are coupled by d-p orbitals hybridization. The transition metal layer and the substrate are also coupled by d-p orbitals hybridization. A method for making graphene-based composite structure is also disclosed.