_{: The electrochemical behaviors of Nd(III) on tungsten electrode and its co-deposition with Al(III) in NaCl-KCl salts at 700 °C were investigated by a series of electrochemical techniques such as cyclic voltammetry, square wave voltammetryand open-circuit chronopotentiometry, and thus Nd-Al alloy was prepared via direct co-deposition of Nd and Al on the inert electrode. The results show thatthe reduction of Nd(III) in NaCl-KCl-NdCl3 melts isa one-step process with three electrons exchanged, and the reaction is anirreversible processcontrolled by diffusionat low scan rate (0.1~0.5V/s) with the calculated diffusion coefficient is approximately 7.6×10^-5cm²/s. After AlCl3introduced into the NaCl-KCl-NdCl3 melts, the curves of cyclic voltammetry, square wave voltammetryand open-circuit chronopotentiometry indicate that three kinds of Nd-Al intermetallic compounds (Nd11Al3, NdAl3 and NdAl2) were formed. It can be deduced that the underpotential deposition of Nd occurs on the tungsten electrode covered with the pre-deposited metal Al from the open circuit chronopotentiometriy. Based on the results of open circuit chronopotentiometriy, the thermodynamic properties of Nd-Al intermetallic compounds were determined by electromotive force measurement at 700 °C, such as the activity of Nd in two-phase coexisting state and relative partial molar Gibbs energies, as well as the standard Gibbs energies ofNd-Al intermetallic compound. Finally, potentiostatic electrolysis was carried out at -2.3Vfor 5h to obtain a product alloys. X-ray diffraction (XRD) and scan electron micrograph (SEM)-energy dispersive spectrometry (EDS) analysis indicated that the obtained alloys were mainly composed of Nd11Al3, NdAl3, NdAl2 and Al phases.}