This paper describes, for the first time, a simple method for the synthesis of uranyl aluminate (URAL) nanoparticles. URAL was prepared by U(VI) hydrolytic precipitation with ammonia at pH = 11 in the presence of mesoporous alumina MSU-X under 20 kHz of sonication followed by annealing of the obtained solids at 800 degrees C. TEM, XAFS, powder XRD, and Al-27 MAS NMR studies revealed that the speciation of uranium in this system strongly depends on uranium concentration. The sample with 5 wt % of uranium yields air-stable nanoparticles (similar to 5 nm) of URAL. Presumably, UO22+ cations in this compound are coordinated with bidentate AlO2- groups. The increase of uranium concentration to 30 wt % causes mostly formation of U3O8 fine particles (similar to 50 nm) and small amounts of URAL.