The unique properties of graphene when coupled to plasmonic surfaces render a very interesting physical system with intriguing responses to stimuli such as photons. It promises exciting application potentials such as photodetectors as well as biosensing. With its semimetallic band structure, graphene in the vicinity of metallic nanostructures is expected to lead to non-negligible perturbation of the local distribution of electromagnetic field intensity, an interesting plasmonic resonance process that has not been studied to a sufficient extent. Efforts to enhance optoelectronic responses of graphene using plasmonic structures have been demonstrated with rather modest Raman enhancement factors of less than 100. Here, we examine a novel cooperative graphene-Au nanopyramid system with a remarkable graphene Raman enhancement factor of up to 10(7). Experimental evidence including polarization-dependent Raman spectroscopy and scanning electron microscopy points to a new origin of a drastically enhanced D-band from sharp folds of graphene near the extremities of the nanostructure that is free of broken carbon bonds. These observations indicate a new approach for obtaining detailed structural and vibrational information on graphene from an extremely localized region. The new physical origin of the D-band offers a realistic possibility of defining active devices in the form of, for example, graphene nanoribbons by engineered graphene folds (also known as wrinkles) to realize edge-disorder-free transport. Furthermore, the addition of graphene made it possible to tailor the biochemical properties of plasmonic surfaces from conventional metallic ones to biocompatible carbon surfaces.