Recent results demonstrating the possibility of preparing graphene-like materials from natural resources such as sucrose (table sugar) and gelatin assembled to silica-based porous solids without a requirement for reducing agents are discussed. The resulting materials show interesting characteristics, such as simultaneous conducting behavior afforded by the sp2 carbon sheets, together with chemical reactivity and structural features, provided by the silicate backbone, which are of interest for diverse high-performance applications. The formation mechanism of supported graphene is still unclear, with further studies being needed to optimize its preparation following these green processes.