Hydrofluxes are hydrated salts with melting points well below that of the dehydrated salt and boiling points well above that of water,a ffording ar eaction medium, in which mild temperatures and pressuresc an be accessedf or the synthesis of materials. Herein, the use of alkali metal hydroxide hydrofluxes for the synthesis of single crystal a-Na 2 NpO 4 is described, and the single crystal X-ray structure of a-Na 2 NpO 4 ,a long with its X-ray absorption spectra and vibrational spectra,i sr eported. The ability to synthesize complex oxideso ft he actinides, in particular,t ransuranium materials, under mild conditions will serve to advance our ability to explore the structureproperty relationships of the fe lements.