We report a simple approach for the production of copper nanoparticles by a wire explosion process that creates different structures in deionized (DI) water versus isopropyl alcohol (IPA) liquid media. In DI water, copper nanoparticles (CNs) are formed, while multi-layer graphene-synthesized copper nanoparticles (MGCNs) with a high degree of graphitization are formed in the IPA liquid media. The nanoparticles have an average diameter ranging from 10 nm to 300 nm and a quasi-spherical morphology. The morphologies and sizes of nanoparticles formed via this method were characterized by high-resolution transmission electron microscopy (HRTEM), field-emission scattering electron microscopy (FESEM), and analysis of dynamic light scattering (DLS). The microstructures and chemical bonding of the nanoparticles were studied by X-ray diffraction (XRD), Raman spectra measurement, and X-ray photoelectron spectroscopy (XPS). This results show an easily reproducible way to synthesize metal-core nanoparticles with multi-layer graphene shells based onto the liquid media used during synthesis. These materials can be used in the field of energy storage and as additives in the near future.