The present disclosure relates to a method for making a graphene/carbon nanotube composite structure. In the method, at least one graphene film is located on a substrate. At least one carbon nanotube layer is combined with the at least one graphene film located on the substrate to form a substrate/graphene/carbon nanotube composite structure. The at least one graphene film is in contact with the at least one carbon nanotube layer in the substrate/graphene/carbon nanotube composite structure. The substrate is removed from the substrate/graphene/carbon nanotube composite structure, thereby forming a graphene/carbon nanotube composite structure.