Dehydrogenation and isomerization of n-butane or isobutane into isobutene over Cr catalysts supported on zeolites were investigated. We found that Cr catalyst supported on H-SSZ-35-type zeolite, having one-dimensional cage-type channel structure, was very effective for this reaction and the yield of isobutene was 5.44% from n-butane and 9.57% from isobutane. In this reaction, it is suggested that dehydrogenation of butanes is accelerated by Cr2O3 loading, and solid acidity of the zeolite support favors isomerization.