Highly active aerobic oxidation of alcohols under mild conditions is achieved by using the catalyst constituted of Au nanoparticles supported on mixed NiAl-oxide derived from its corresponding layered double hydroxide. Besides the contribution of electronic interaction, the enhanced catalytic property of the Au catalyst is mainly attributed to the synergistic effect between the Au and the support on reaction mechanism. The unique support with loading Au nanoparticles comes through structural interconversion between the mixed oxide and the layered double hydroxide upon the water exchange during the reaction, which is beneficial to the fast removal of water from the Au surface and then accelerates the restore of the active sites of Au for oxidation of alcohols. (C) 2014 Elsevier B.V. All rights reserved.