. Al-pillared rectorites (Al-REC) were synthesized from natural calcium rectorite through the exchange of inter-lamellar ions with hydroxyalumina polycations. Furthermore, the morphology, composite structure and pore properties of such composite materials were investigated by Powder X-ray Diffraction (XRD), Fourier Transformation Infra-red Spectra (FTIR) and Nitrogen Adsorption-Desorption Isotherms. The products retain their layered structure and their pore structures are a slit-shaped pore between plate-like particles. The resultant products possess BJH pore volume as large as 0.04cm3g-1, high BET specific surface area of over 100m2g-1, narrow pore size distribution in the mesopore region of 7-9nm after thermal treatment at 300 °C.