Organo-functional silanes which were able to form chemical bonds with kaolinite and could also have an affinity to the materials of concern here, were studied by the sol-gel process. Polymethacrylate with trialkoxy silyl functional groups were prepared, hydrolysed and co-condensed with kaolinite. The progress of the hydrolysis, which proceeded very slowly, was followed by Karl-Fischer titration. Thermal behavior was investigated by differential thermal analysis. The extent of the reaction leading to network formation was qualitatively followed by Fourier transform-infrared spectroscopy and X-ray diffraction. Free-radical polymerization was carried out ultrasonically in the presence of a catalyst. Trimethoxy silane end-capped silane was found to be covalently bonded to kaolinite. The copolymers, with various amounts of kaolinite, were then hydrolysed and co-condensed in the presence of a catalyst to yield sol-gel materials which have a controllable combination of properties of both the polymer and kaolinite.