Disclosed are a method of growing a high-quality single layer graphene by using a Cu/Ni multi-layer metallic catalyst, and a graphene device using the same. The method controls and grows a high-quality single layer graphene by using the Cu/Ni multilayer metallic catalyst, in which a thickness of a nickel lower layer is fixed and a thickness of a copper upper layer is changed in a case where a graphene is grown by a CVD method. According to the method, it is possible to obtain a high-quality single layer graphene, and improve performance of a graphene application device by utilizing the high-quality single layer graphene and thus highly contribute to industrialization of the graphene application device.