A functionalized surfactant, GME-N-C10 containing a C=C double bond, was synthesized to modify clays such as montmorillonite (MMT) and mica for the preparation of organic-inorganic composite resins via radical photoinduced polymerization. As revealed by X-ray diffraction (XRD) analysis of the organophilic samples, the synthesized surfactant was successfully intercalated into the layers of clay by its full molecular length and such an intercalation generated a paraffin-like structure in the modified clays. By forming the C-C bonds between surfactants and oligomers/monomers during subsequent radical photoinduced polymerization, the hybrid comprising organophilic clay/oligomers/monomers became an intercalated nanocomposite resin. The thickness of the dispersed lamellae was less than 100 nm, as revealed by transmission electron microscopy (TEM). For the composite sample containing 5.0 wt.% of organophilic clay, the decomposition temperatures raised at least 15°C; the transmittance detected by UV-visible spectrometer showed a less than 15% loss in the visible light region but a satisfactory transparency was still retained, and the degree of moisture absorption decreased from 3.4% to about 1% due to dispersive organophilic clay in the polymer matrix.