Crystalline ZnO and ZnO 2 nanoparticles (NPs) were prepared in one-pot oil-in-water (O/W) microemulsion media at room temperature by adding an aqueous solution of sodium hydroxide (followed by H 2 O 2 in the case of synthesis of ZnO 2 ) to the O/W microemulsion containing a Zn(II) organometallic precursor dissolved in the oil phase. After calcination of ZnO 2 NPs, ZnO NPs were also obtained, and their characteristics were compared with those of ZnO NPs prepared directly in O/W microemulsion. The materials were characterized by X-ray diffraction, scanning electron microscopy, and high-resolution transmission electron microscopy. Nanostructured ZnO materials have attracted a lot of attention in recent years because of their optical, electrical, and chemical properties, as well as their low toxicity. These materials are n-type semiconductors with a band gap of 3.37 eV and an exciton binding energy of 60 meV; in addition, they exhibit efficient UV-stimulated emission 1 at room temperature. Nanostructured ZnO has great potential for use in a wide range of applications, for example, in phosphors, 2,3 varistors, 4a,4b gas sensors, 57 UV absorbers, 8 and antimicrobial agents, 9 and more recently, in solar cells.