A method of synthesizing alkali uranium fluorophosphate crystals. The method includes combining a uranium-based feedstock with a mineralizer solution. The mineralizer solution includes an alkali nutrient, a phosphate, and a fluoride. The feedstock and mineralizer solution are pressurized and a thermal gradient applied thereto such that a first portion of the feedstock and the mineralizer solution is heated to a temperature that is greater than a temperature of a second portion of the feedstock and the mineralizer solution. Uranium nutrient enters the mineralizer solution from the feedstock in the first portion and uranium nutrient precipitates to spontaneously form crystals in the second portion.