With the expansion of the automobile market, the demand for Nd as an essential rare earth material for automobile motors is rapidly increasing. Research on the calcio-thermic reduction process between Nd2O3 and calciumbased alloys has been extensively studied in order to manufacture Nd. In this study, Ca-Cu, as a reducing for Nd2O3, was prepared by electrolysis in CaCl2 molten salt. Cu wire and graphite were employed as a working electrode and a counter electrode for electrolysis reaction, respectively. The reference electrode was manufactured by putting Ag wire in a mixture of AgCl and CaCl2 at a ratio of 1:99 mol%. The cyclic voltammetry results showed that the deposition of Ca2+ on the surface of working electrode was observed from a potential of -1.8 V, and the reduction potential of Ca2+ decreased as the reaction temperature increased. The diffusion coefficient of Ca2+ calculated by the chronoamperometry experiment was found to be 5.4(±6.8)×10-6 cm2/s. In addition, Ca-Cu liquid alloy was prepared by applying a constant potential to Cu electrodes. The element ratio of Ca-Cu alloy formed by applying a potential of -2.0 V was found to Ca:Cu=1:4.