The preparation of UO2 microspheres by the Hydrolysis Process is based on the solidification of droplets of a concentrated uranyl " nitrate solution in hot oil. The uranyl nitrate is complexed by urea and partly hydrolized by adding solid hexamethylentetramine. The temperature depending solidification reaction of the metastable solution is a continuous polymerisation of [(U02 (OH)2)n UO2]2+ ions forming kolloidal UO2(OH)2. The crystallite size of the spherical gel particles is increased by washing with hot water. Heat treatment of the washed and dried particles in reducing atmosphere leds to UO2 with excellent sintering behaviour. The process was also successfully applied to the preparation of ThO2 and (U,Th)O2 microspheres