A series of Al100-xCr(x) alloys (x = 11, 14, 25, 41) have been electrodeposited from a 2AlCl3-NaCl melt containing approximately 0.1 mol/liter Cr2+ at 175-degrees-C. The alloy composition and structure were functions of the deposition potential. Depending upon the specific deposition parameters, the deposit microstructure consisted of the zeta-Al8Cr5 compound, metallic glass, and/or an fcc phase. The Cr2+ concentration was monitored by voltammetric analyses of the quasi-reversible Cr2+/Cr3+ couple, carried out at high sweep rates due to the limited solubility of Cr3+. Specular Al100-xCr(x) alloys were also deposited from a room temperature 2AlCl3-TMPAC melt.