The electrodeposition of aluminum in the molten binary AlCl3‐NaCl system has been studied. The properties of the aluminum deposited layers varied with the preelectrolysis process of melts, the operation temperature, the current density, and the composition of electrolytes. The aluminum was unable to deposit from a basic AlCl3‐NaCl melt; whereas by increasing the concentration of A1C13, a denser, more compact and uniform deposited layer was obtained.