In this work, nanocomposite adhesives obtained using an organically modified montmorillonite (OMM) in a polyurethane matrix were studied. The basal distance of OMM before and after mixing with the polyol and after curing was characterized by X-Ray diffraction. The viscosity of polyols-OMM systems was studied as function of shear rate in a cone-plate rheometer in order to correlate the viscosity with the aggregation state of OMM. A simple model accounting for an apparent increase of rheological units size associated with the intercalation of macromolecules into OMM galleries is proposed. Curing was performed at room temperature for 1 week. The basal distances of crosslinked PU nanocomposites were obtained by X-ray diffraction. The glass transition temperature, T-g, of PU nanocomposites, as measured using differential scanning calorimetry, increases with increasing volume fraction of OMM. Finally, the permeability to oxygen and water vapor of polyurethane clay-nanocomposites was measured. The gas permeation through the composites was correlated to the volume fraction of the impermeable inorganic part of the OMM. POLYM. ENG. SCI., 49:1708-1718, 2009. (C) 2009 Society of Plastics Engineers