ZnAl2O4 and ZnO nanostructure particles and in situ crystallization of zinc aluminate and zinc oxide coating layers on sintered alpha-Al2O3 and gamma-Al2O3 granules by the microwave-assisted combustion method were investigated. For powders, the effects of solution pH value and for coated samples the influence of support type on the structure, microstructure, and photocatalytic activity of powders were studied. Results showed that variation of synthesis pH value caused to considerable change in agglomeration, specific surface area, obtaining up to 88 and 92% yields for zinc aluminate and zinc oxide nanoparticles, respectively. gamma-alumina granules were more appropriate supports than the alpha-alumina ones because of the better photocatalytic activities and lower extent of the attritions for both zinc aluminate and zinc oxide coating layers.