Low-temperature synthesis of multilayer graphene (MLG) is essential for combining advanced electronic devices with carbon materials. We investigated the vapor-phase synthesis of MLG by sputtering deposition of C atoms on metal-coated insulators. Ni, Co, and Fe catalysts, which have high C solid solubility, enabled us to form MLG at 400 °C. The domain size and surface coverage of MLG were determined by the supplied amount of C atoms and the thickness of the metal layer associated with the solid solution amount of C. An average domain size of 2.5 μm and surface coverage of approximately 50% were obtained for a 1 μm thick Ni layer. Transmission electron microscopy demonstrated the high crystalline quality of the MLG layer despite the low processing temperature. Therefore, this simple sputtering technique has great potential for integrating graphene-based devices on various platforms.