Carbon nanotubes (CNTs) are excellent multifunctional materials in terms of mechanical robustness, thermal, and electrical conductivities. These multifunctional properties, as well as the small size of the structures, make CNTs ideal building blocks in developing nanocomposites. However, the matrix materials and the fabrication processes are critical in achieving the expected multifunctional properties of a CNT-reinforced nanocomposite. This paper has proved that electrochemical co-deposition of a metallic nanocomposite is a good approach for achieving good interfacial bonding between CNTs and a metallic matrix. Good interfacial bonding between a single-walled carbon nanotube (SWCNT) and a copper matrix has been verified by enhanced fracture toughness (increased stickiness) and a shift in the Raman scattering spectra. For the Cu/SWCNT nanocomposite, the radial breath mode (RBM) has disappeared and the tangential or G-band has shifted and widened, which is an indication of better energy transport.