Organo-kenyaite that interlayer surface bonded chemically with amine groups were prepared by siliation 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 41.4-51.2 Å. 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. This result should offer a promising route leading to the preparation of organo-layered materials that a various functional group are bonded chemically in interlayer surface.