Graphene has attracted an enormous amount of interest recently because of its unique electronic, optical, mechanical, and other properties. We report a promising method for producing single-layer graphene fully covering an entire substrate at low temperature. Single-layer graphene sheets have been synthesized on a whole 2 cm x 2 cm nickel (Ni) film deposited on a highly oriented pyrolytic graphite (HOPG) substrate by heating the Ni/HOPG in a vacuum. The carbon atoms forming our graphene are diffused from the graphite substrate through the nickel template. Our results demonstrate how to control the amount of carbon atoms for graphene formation to yield graphene films with a fine controlled thickness and crystal structure. Our method represents a significant step toward the scalable synthesis of high-quality graphene films with predefined thickness and toward realizing the unique properties of graphene films.