By simply coating graphene films on Au nanoparticles, the optical properties of the hybrid films are investigated. It is found that the coverage of a monolayer graphene film leads to a decreased transmittance of up to 15.8% in the visible range, much higher than the 2.3% transmittance loss for intrinsic graphene. At the same time, the plasmonic resonance of the hybrid films experiences a red-shift in resonance frequency and a broadening in the transmission dip. By means of finite element simulations, these observations are attributed to strong light–matter interaction at the interface between graphene and Au nanoparticles, as indicated by the increased absorption cross section and higher electric field intensity. The electron transfer between graphene and Au nanoparticles is confirmed by high resolution X-ray photoelectron spectroscopy studies. Furthermore, the enhanced electromagnetic hot spots at the interface between graphene and Au nanoparticles make such graphene–Au nanoparticle hybrid films cost-effective and high-performance surface-enhanced Raman scattering substrates for detecting organic molecules such as rhodamine-6G, for which an enhancement factor of [similar]107 is achieved.