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Graphene has attracted significant attention due to its excellent electrical, optical, mechanical and thermal properties. In the paper, we report a simple and efficient growth method of multilayer graphene using a metal-catalyzed crystallization of diamond-like carbon (DLC) by thermal annealing without any extraneous carbon sources. The Ni/DLC/Si multilayered structure was fabricated on silicon substrate at room temperature (RT) and then was thermally annealed. Multilayer graphene was formed on the nickel surface after cooling down to RT by the analysis of Raman spectra. The quality of the multilayer graphene is comparable to chemical vapor deposition methods (CVD). This method of synthesizing graphene sheets with DLC films provides an important way toward the integration of DLC-based electronic devices with graphene.