This paper reports synthesis and characterization of polyurethane-Urea (PU-urea) and the nanocomposites derived from the PU-Urea with silicate clays. Organophilic montmorillonite cotreated by cetyl trimethyl ammonium bromide (CTAB) was synthesized and used to prepare PU-urea/montmorillonite nanocomposites coatings. PU-ureas were prepared from polyethylene glycol (PEG), polypropylene glycol (PPG), trimethylol propane (TMP), and 4,4'-diphenylmethane diisocyanate (MDI) by reacting excess diisocyanate with polyether glycols. The excess isocyanate of the prepolymers was cured with atmospheric moisture. The synthesized moisture Cured PU-Urea and nanocomposites were characterized by Fourier transform infrared (FTIR) spectroscopy, thermogravimetric analysis (TGA), differential scanning calorimetric (DSC), and angle resolved X-ray photoelectron spectroscopy (AR-XPS). The thermal stability of the PU-Urea nanocomposites was higher relative to the mother PU-Urea films. DSC results showed a slight enhancement in the soft segment glass transition temperature after 3 wt % clay loading. The surface properties showed ail enrichment of the soft segment toward the surface. Ail enhancement in the hard segment composition in the nanocomposite coatings has resulted in enhancing the phase mixing process. (c) 2006 Wiley Periodicals, Inc.