The modification of Cu–Zn catalysts with low amount of Al and Ga (Al+Ga = 3%) was investigated and data corresponding to its influence on the decomposition of the calcined precursors and on the nanomorphology and surface concentration of reduced catalysts were presented in this contribution. The data presented here are supplementary material of the catalysts presented in the research article “Structure and activity of Cu/ZnO catalysts co-modified with aluminium and gallium for methanol synthesis” published in Catalysis Today [1]. Keywords: Methanol synthesis, Copper, Zinc, Gallium, Catalysts