In this study, anionic surfactant and silane modified hydrotalcites were synthesized through a soft chemical in-situ method. The resulting materials were characterized using X-ray diffraction (XRD), high-resolution thermogravimetric analysis (HRTG), Fourier Transform Infrared spectroscopy (FTIR), Transmission Electron Microscopy (TEM), Scanning Electron Microscopy (SEM) and N2 adsorption-desorption. The Mg-Al hydrotalcite (LDH) and the only surfactant modified hydrotalcite (LDH-2) display similar XRD patterns while both surfactant and silane modified hydrotalcite (LDH-3) shows two distinct series of reflections, corresponding to hydrotalcite and smectite-like materials, respectively. The smectite-like materials shows a series of regular (001) reflections with d001=12.58 Å. Further supporting evidence was obtained from FTIR and TG, for example, the vibration at 1198 cm-1 corresponds to Si-O-Si stretching mode and the mass loss at ca. 861 oC to dehydroxylation. In LDH-2, the loaded surfactant are located in both the interlayer space and inter-particle pores with a “house of cards” structure as supported by FTIR, TG and N2 adsorption-desorption isotherms. Both electron microscopy (SEM and TEM) micrographs and N2 adsorption-desorption isotherms show that in-situ modification with surfactant and silane has a significant influence on the morphology and porous parameters of the resulting hydrotalcite materials.