Vanadia impregnated iron-pillared montmorillonites with different weight percentages of vanadia have been prepared. Subsequent characterization by XRD, FT-IR, surface area and pore volume measurements was carried out. Acidity was determined by three independent techniques, namely thermogravimetric desorption of 2,6-dimethylpyridine, spectrophotometric monitoring of adsorption of perylene and temperature-programmed desorption of ammonia. Conversion of cumene in the vapor phase has been performed as a test reaction of acidity. Aniline methylation was carried out to check the catalytic efficiency of the solids.