Composite materials with graphene-augmented carbon reinforcement fibers having a graphene film wrapped about one or more carbon fiber filaments. The graphene film is wrapped about the carbon fiber filaments in a spiral orientation and has amine groups formed on an outer surface of the graphene film and epoxide groups formed on at least one edge of the graphene film. The amine groups are formed in a functionalized area on the outer surface of the graphene film that is within about 10 microns from the at least one edge of the graphene film. The graphene film may also have holes formed through the graphene film. The graphene film may be wrapped around a single carbon fiber filament, a substantially cylindrical bundle of about 19 carbon fiber filaments, or a substantially rectangular bed of carbon fiber filaments formed from a plurality of carbon fiber tows.
