Size characteristics, structure, and spectral and luminescent properties of nanoparticles fabricated by laser ablation of zinc metal targets in water and ethanol are experimentally investigated upon excitation by Nd:YAG-laser radiation (1064 nm, 7 ns, and 15 Hz). It is demonstrated that zinc oxide nanoparticles with average sizes of 10 nm (in water) and 16 nm (in ethanol) are formed in the initial stage as a result of ablation. The kinetics of the absorption and luminescence spectra, transmission electron microscopy, and x-ray structural analysis demonstrate that during long storage of water dispersions and their drying, nanoparticles efficiently interact with carbon dioxide gas of air that leads to the formation of water-soluble Zn(CO3)(2)(OH)(6). In ethanol, Zn oxidation leads to the formation of stable dispersions of ZnO nanoparticles with 99% of the wurtzite phase; in this case, the fluorescence spectra of ZnO nanoparticles change with time, shifting toward longer wavelength region from 550 to 620 nm, which is caused by the changed nature of defects.