A reprocessing process of spent nuclear fuels for roughly separating U and U—Pu from FP, TRU and the like in a nitric acid solution of spent nuclear fuels by utilizing phenomenon of cocrystallization of hexavalent U and Pu. For example, spent nuclear fuels are sheared and dissolved in nitric acid, and insoluble residues in the nitric acid solution are removed. Then, a nitric acid concentration in the solution is adjusted and a valence of Pu in the solution is adjusted to tetravalence. The solution is then cooled to crystallize uranyl nitrate hydrate crystals and separated into the crystals and a mother liquor, and the separated crystals are recovered as a U product. Then, a nitric acid concentration in the separated mother liquor is adjusted and a valance of U and Pu in the mother liquor is adjusted to hexavalence, and the mother liquor is cooled to crystallize uranyl-plutonyl nitrate hydrate crystals which are separated and recovered as a U—Pu mixed product.