a b s t r a c tThis study investigated the use of novel organic solvent baths for the electrodeposition of aluminum at near-ambient temperatures. It was found that Al metal can be electrodeposited from baths that were composed of 1,3-dimethyl-2-imidazolidinone (DMI) and AlCl 3 , with an AlCl 3 concentration greater than 50 mol%. IR spectroscopy indicated that Al 2 Cl 7 − ions were present in the baths that contained >50 mol% AlCl 3 , where the electrodeposition of Al occurs from Al 2 Cl 7 − ion. The DMI/AlCl 3 baths with AlCl 3 concentrations between 59 and 64 mol% retained a single liquid phase without precipitation at 25 • C, and therefore, they can be used for Al electrodeposition near room temperature. Smooth Al films could be obtained by galvanostatic electrodeposition at 40 • C using a DMI/AlCl 3 bath with the addition of a trace amount of 1,10-phenanthroline.