Spherical UO nanoparticles were firstly prepared by reactions of 0.01 or 0.05 M of UO(NO) with 0.025-0.04 or 0.5-5.0 M of hydrazine at 160 °C, respectively. However, UO formed when 0.01 M of UO(OAc) was used for reaction with 0.025-0.04 M of hydrazine. When ethylenediamine was used to react with 0.025-0.05 M UO(NO) or 0.025 M UO(OAc), unknown purple compounds formed at lower concentrations of ethylenediamine and the products became unique UO at 10.0 and 7.5 M ethylenediamine, respectively. These results demonstrated that reaction conditions significantly affect the products of uranium oxides prepared by hydrothermal methods.