Recent studies indicate that a template method for creating Al-pillared clays, in which surfactant micelles foster the creation of a homogeneous mesoporous network within the pillar, effectively enhance catalyst performance and adsorbent properties. No studies, however, have described the relative effects of the surfactant concentration and Al content on the textural and acidic properties and on the catalytic activity of the Al-pillared clays. The purpose of the present study was to fill this gap, using the isomerization of 1-butene as the test process for catalytic activity. Modified pillared clays (MPC) were prepared from a synthetic clay, TS-1, using different amounts of a non-ionic surfactant (Igepal CO-720) and a fixed concentration of a solution containing the Al polycation [Al13O4-(OH)24]7+. MPC with a fixed amount of surfactant and different amounts of Al were also prepared. The catalysts were characterized by X-ray diffraction (XRD), X-ray fluorescence (XRF), temperature-programmed desorption of ammonia, 27Al magic-angle spinning nuclear magnetic resonance (27Al MAS NMR), and N2 adsorption/desorption isotherms. Isomerization of 1-butene at 250°C was used to test the catalytic activity. Analyses by XRD and XRF showed that the synthesized solids were amorphous and that the amount of pillaring by Al increased with the amount of Al complex used. Interestingly, the surface area and pore volume were directly proportional to the amount of surfactant employed and decreased with increasing amounts of Al pillaring. All solids showed activity for 1-butene isomerization, with a maximum conversion of ~75%. Only cis- and trans-2-butene were observed. The absence of isobutene suggested that acid sites of moderate strength were formed, in agreement with the results obtained from the desorption of ammonia.