A sodium bentonite (montmorillonite-based layered silicate clay) was organically modified with cetyl trimethyl ammonium bromide (cetrimide), using different clay/water ratios-but the same clay/cetrimide ratio-to suspend the bentonite clay and perform its organophilization. Infrared spectroscopy and thermogravimetric analysis indicated the incorporation of organic modifier into the bentonite. Wide-angle X-ray scattering showed that the incorporation of surfactant significantly increased the interlayer spacing in the bentonite for all concentrations studied. It was found that clay/water ratio employed during the modification affects neither the amount of organic salt incorporated nor the interlayer spacing in the organobentonites, but influences its degree of structural disorder. Lower clay/water ratios resulted in a more disorderly structure, as established by the decrease of the areas under the X-ray peaks as the clay/water ratio diminishes. The modified bentonites were melt compounded with maleic anhydride-grafted polypropylene. X-ray diffraction patterns of the hybrids revealed that the more disorderly organobentonites were better dispersed in the polymer matrix, indicating that, in the present system, the structure of polymer nanocomposites obtained were affected by the clay/water ratio used in organobentonite preparation. POLYM. ENG. SCI., 49:1696-1702, 2009. (C) 2009 Society of Plastics Engineers