3-aminopropyltriethoxysilane grafted montmorillonites were synthesized with montmorillonite, acidactivated montmorillonites and 3-aminopropyltriethoxysilane in ethanol-water mixture. The resulting products were investigated using Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction (XRD), thermogravimetric analysis (TG). XRD patterns demonstrated that silane was intercalated into the montmorillonite gallery, indicated by increasing basal spacings. These intercalated silanes probably adopt bilayer arrangement models within the montmorillonite and acid-activated montmorillonites interlayer spaces. TG and DTG curves indicate that acidification results in a decrease of the thermal stability of the resultant montmorillonites. Silane grafting leads to a surface property transformation of montmorillonite from hydrophilicity to lipophilicity and an increase of the thermal stability of the condensed silanes.