This chapter deals with the study of the electrolysis synthesis of copper matrix nanocomposites developed for the fabrication of nanoparticulate Cu-bimetals. In this chapter, we describe the successful synthesis of Cu matrix nanocomposites by the electro-deoxidation method. We think that this approach will make it possible to realistically integrate a series of copper-bimetals. This study makes a significant contribution to the literature because this method opens novel opportunity to the design of nanocomposite materials. Particularly, this opens up prospects for designing the new materials from immiscible metallic elements, which is the main topic in designing of alloys as well as materials science progression.