In an effort to develop new electrical insulation materials, four different kinds of organically modified layered silicate were incorporated into an epoxy matrix to prepare nanocomposites for electrical insulation. Five wt% of organically modified layered silicates were processed in a planetary centrifugal mixer in an epoxy matrix, and the thermal, mechanical, and electrical properties of the cured epoxy/layered silicate were investigated. The morphology of the nanoscale silicate dispersed in the epoxy matrix was observed using transmission electron microscopy, and the interlayer distance was measured by wide-angle X-ray scattering diffraction analysis.