Abstract: Using natural Na montmorillonite as the host clay, porous silicapillared montmorillonites (SiPILC) were prepared by the template synthesis method. Furthermore, the texture and structure of such composite materials were investigated by using modern several physicochemical techniques such as powder X-ray Diffraction (XRD), X-ray Fluorescence (XRF), Fourier Transformation Infrared Spectra (FTIR), and N2 adsorption/desorption measurements. The results reveal that tetrathylorthosilicate (TEOS) agent has been successfully intercalated into the montmorillonite and the characteristic d001 spacing of SiPILC increases from 1.28nm to 3.15nm. The resultant products with large gallery height possess BJH pore volume as large as 0.30cm3/g, remarkably high BET specific surface area of over 592.0m2/g, pore size distribution in the mesopore region 3.3nm~4.3nm after thermal treatment at 800℃.