Dehydrogenation of isobutane to isobutene over supported gallium oxide microspherical catalysts was investigated in a fluidized-bed reactor. A partially crystallized nanostructured aluminum hydroxide-oxide, which is a product of gibbsite centrifugal thermal activation (CTA) obtained using a CEFLAR technology, was used as a catalyst support. The structural and textural properties of Ga2O3/Al2O3 catalysts were characterized by a range of techniques including XRD, N2-physisorption, TPD of NH3 and CO2, IRS of adsorbed pyridine, and selective adsorption of a series of acid–base indicators. A Ga–Al oxide catalyst exhibited a stable performance close to activity of Cr–Al oxide catalysts not containing soluble hexavalent chromium. Upon addition of Cr2O3 (6 wt % of Cr), in amounts lower than in an industrial chromia/alumina catalyst (10.9% Cr), and 1% ZrO2 to 6%Ga/Al2O3 catalytic activity in isobutane dehydrogenation reaches the performance of the industrial KDM catalyst (“Sintez”, Russia).