Organo layered silicate that interlayer surface bonded chemically with amine groups were prepared by sililation of γ-aminopropyltriethoxysilane (APS) with interlayer Si-OH groups in the presence of gallery expander dodecylamine (DDA) in ethanol. The interlayer surface sililation were performed by the vaporization of ethanol from the slurry composed of APS, DDA, H-kenyaite and ethanol. XRD analysis of dried-powder resulted in well-ordered large d-spacing of 4.1-5.2 nm. ²⁹Si solid state NMR showed a substantial increase in the relative intensity Q⁴ signals due to newly formed Q⁴ units by the sililation of interlayer surface Si-OH groups. The properties of nanocomposite were measuered by TEM and SAXS. The distance in the interlayers was expanded up to 5 ~ 6 nm. Nanocomposite in well exfoliated and dispersed by extension of interlayers caused by the intercalation of epoxy resin. This result should offer a promising route leading to the preparation of organo-layered materials that a various functional groups are bonded chemically in interlayer surface.