In this article, we reported a spin successive ionic layer adsorption and reaction (SILAR) method for the first time. ZnS thin films were deposited by spin SILAR using ZnCl2 and Na2S aqueous precursor solutions at room temperature and atmosphere pressure. The optical, structural, and morphological characterizations of the films were studied by scanning electron microscopy, atomic force microscopy, transmission electron microscopy, X-ray photoelectron spectroscopy, and UV/visible spectroscopy. Smooth (average roughness < 3 nm), uniform, and highly transparent ZnS (transmittance of over 90% in the visible band) thin films could be successfully deposited using this technique with shorter cycle time and much less solvent usage. (C) 2010 The Electrochemical Society. [DOI: 10.1149/1.3428742] All rights reserved.