Control over the film-substrate interaction is key to the exploitation of graphene’s unique electronic properties. Typically, a buffer layer is irreversibly intercalated “from above” to ensure decoupling. For graphene/Ni(111) we instead tune the film interaction “from below”. By temperature controlling the formation/dissolution of a carbide layer under rotated graphene domains, we reversibly switch graphene’s electronic structure from semi-metallic to metallic. Our results are relevant for the design of controllable graphene/metal interfaces in functional devices.
