Various mesoporous chromia alumina catalysts were prepared by five different methods based on a metal-organic framework MIL-101 and their catalytic performances over isobutane dehydrogenation were investigated. The highly dispersed chromium species were produced on catalyst KCrAI-I1 with largest specific surface area of 198 m2-g-1 prepared with aluminium isopropoxide (Al(i-OC3HT)3) by ultrasonic im- pregnation method. However, the catalyst KCrAI-I2 synthesized by stirring impregnation possessed crystalline a-Cr203 phase, which was poorly dispersed. Two types of Cr-rich and Al-rich CrzA12_zO3 solid solutions, designated as CrAI-I and CrAI-II phase, were formed over the catalysts KCrAI-I3 (prepared by Al(i-OC3HT)3 with nitric acid regulation), KCrA1-C4 (prepared by aluminium chloride hexahydrate) and KCrA1-N5 (prepared by aluminium nitrate nonahydrate). Catalytic evaluation results revealed that KCrAI-I1 exhibited the high isobutane con- version due to its highly dispersed chromium species. However, KCrAI-I3, KCrA1-C4 and KCrA1-N5 showed the higher isobutene selectivity (95.2%-96.4%) on account of the formation of chromia alumina solid solutions in the catalysts. Moreover, the solid solution over the chromia alumina catalysts could greatly suppress the coke formation.