A comparative study on acid and hydrothermal methods as ways to reduce interlamellar charge has been carried out on a vermiculite. This study showed that the application of the hydrothermal treatment as a previous step to pillaring the vermiculites, reported here for the first time, is a new route to obtain the porous material with a particular interest as heterogeneous catalysts, starting from mineral clays with a high density of charge. Modified clays have been characterized by atomic absorption, emission spectrograph, X-ray diffraction, cation-exchange capacity, total acidity, infrared spectroscopy (DRIFT), and nitrogen adsorption. The results have shown that all solids have been structurally modified. However, acid and hydrothermal methods showed different behavior. For the vermiculite, the hydrothermal treatment did not produce major differences in terms of the crystalline structure, whereas the acid method caused severe structural damage. The catalytic properties have been tested over Pt-impregnated samples (1%) using the hydroisomerization of heptane. important catalytic activity was established for all solids with high selectivity regarding the isomer products.