Neodymium was electrochemically deposited from NdF3–LiF–Nd2O3 molten salt electrolyte onto the Mo electrode at temperatures close to 1273 K. Cyclic voltammetry and chronoamperometry measurements were the applied electrochemical methods. Metallic neodymium is obtained by potentiostatic deposition. The optical microscopy and XRD were used to analyze the electrolyte, the working electrode surface, and the deposit on the electrode. It was established that Nd(III) ions were reduced to Nd metals in two steps: Nd(III) + e− → Nd(II) at potential ≈−0.55 V vs. W and Nd(II) + 2e− → Nd(0) at ≈−0.83 V vs. W. Both of these processes are reversible and under mass transfer control. Upon deposition under the regime of relatively small deposition overpotential of −0.10 V to −0.20 V, and after the electrolyte was cooled off, Nd metal was observed at the surface of the Mo electrode. CO and CF4 were gases registered as being evolved at the anode. CO and CF4 evolution were observed in quantities below 600 ppm and 10 ppm, respectively.