Zirconium pillared montmorillonite and vermiculite clay catalysts have been prepared by different methods of intercalation. The catalysts were characterized by XRD, nitrogen adsorption, Infared (IR) and differential scanning calorimetric (DSC) studies. Toluene methylation activity is found to depend on the preparative method and zirconium concentration of the catalysts. The results indicate a direct correlation between the density of Lewis acid sites and toluene methylation activity.