Abstract: A method of producing uranium chloride. The method comprises combining a uranium feedstock, a chlorinating agent, and a metal salt in a reaction vessel to form a reaction mixture. The reaction mixture is heated to a temperature of from about 600° C. to about 850° C. to form uranium chloride or a uranium chloride eutectic mixture. The uranium chloride or the uranium chloride eutectic mixture is separated from the reaction mixture. A composition comprising uranium chloride or a uranium chloride eutectic mixture at a purity of greater than about 99.9 is also disclosed, as are additional methods of producing uranium chloride.