Hybrid organic/inorganic nanocomposites composed of zinc hydroxide and surfactant molecule, and/or zinc oxide nanoparticles were fabricated using pulsed laser ablation of zinc in aqueous solutions of various surfactants. A Zn plate was ablated by a pulsed Nd:YAG laser in four types of surfactant solutions with different concentrations. Zinc oxide nanoparticles with average diameter of 10–40 nm were obtained in cationic, amphoteric and nonionic surfactant solutions. Unique layered organic/inorganic nanocomposites composed of zinc hydroxide layers and surfactant molecules were obtained in aqueous solutions of the anionic surfactants, sodium alkyl sulfate (C n H2n+1SO4 -·Na+). The carbon number, n, in the alkyl sulfate family is very important for the formation and structure of the layered nanocomposites. The layered organic/inorganic nanocomposite can be obtained only in the specific sodium alkyl sulfates (n = 12, 13, 14 and 16) and the layer spacing of the nanocomposites increased with n from 26.8 Å to 42.0 Å. It is shown that the structures of ZnO nanoparticles and layered organic/inorganic nanocomposites can be controlled by the type of surfactants in solution.