Small amounts of gallium ions were added to y-alumina and their influence on the structural properties of the system Co-(Mo)/y-Al203 was studied. It is shown that, due to the presence of Ga3+ ions, a "surface" spinel CoAl204 is formed with a larger amount of Co2+ in tetrahedral sites as compared to the spinel formed on gallium-free alumina. A decrease of the segregated Co304 is also observed. A possible effect of gallium ions on molybdenum is discussed. It is also reported that different preparation methods (single or double impregnation) lead to the formation of different surface species. Cobalt aluminate, molybdate monolayer, and Co3O4, depending on the Co content, are formed on doubly impregnated specimens. Cobalt aluminate and cobalt molybdate are the main species formed on singly impregnated specimens. Finally brief consideration is given to how the Co and Mo species, present in the oxide form, change in the sulfided form.