Smectite-type materials which contain different divalent cations (Ni2+, Co2+, Mg2+, and Zn2+) in octahedral sheets have been synthesized and characterized by pyridine adsorption and catalytic effectiveness for the isomerization of 1-butene. All smectite-type materials examined have Lewis acid sites; however, the activity values for the isomerization of 1-butene significantly depend on the divalent cation species included. Nickel-containing smectite-type catalysts are stable and the most active among the smectite catalysts.