Metal-catalyzed crystallization of amorphous carbon to graphene by thermal annealing is demonstrated. In this “limited source” process scheme, the thickness of the precipitated graphene is directly controlled by the thickness of the initial amorphous carbon layer. This is in contrast to chemical vapor deposition processes, where the carbon source is virtually unlimited and controlling the number of graphene layers depends on the tight control over a number of deposition parameters. Based on the Raman analysis, the quality of graphene is comparable to other synthesis methods found in the literature, such as chemical vapor deposition. The ability to synthesize graphene sheets with tunable thickness over large areas presents an important progress toward their eventual integration for various technological applications.