As a step in the development of a new reprocessing method for spent nuclear fuels, a fluoride volatility pilot plant has successfully demonstrated the recovery of uranium as uranium hexafluoride from unirradiated uranium-zirconium and uranium-aluminum alloy fuels. The process involves the separation of the alloying metal as a volatile chloride by reaction with hydrogen chloride in a fluid-bed reactor, followed by reaction of residual solid uranium chlorides with hydrogen fluoride and then with fluorine gas to effect recovery of uranium hexafluoride. In tests involving the processing of up to 30 kg of simulated fuel, uranium recoveries of > 99% were achieved. The volatile zirconium and aluminum chlorides are converted to solid oxides for waste disposal by reaction with steam in a fluid-bed reactor.