Abstract: ADU (ammonium diuranate) is prepared in particle form directly by reacting ammonium gas with liquid droplets of atomized uranyl compound solutions. Generation of liquid filtrate is prevented by using concentrated solutions of uranyl compounds as feed solutions, or drying the wet ADU particles formed before their settlement when a feed of low concentration is used. The ADU particle thus prepared is finely divided and easy-handling. No filtration operation is necessary in the preparation. The UO.sub.2 powder consequently obtained after calcining and reduction has consistent quality from batch to batch and has good pelletizing and sintering properties. Uranium dioxide with low fluorine content can be prepared from uranyl fluoride solution. Gadolinium-uranium oxide can also be prepared with the present method using an aqueous mixture of gadolinium nitrate and uranyl nitrate as a feed solution.