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Mixed PMoV heteropoly acids with Keggin structures H3+xPMo12–xVxO40 (x = 1–6) and modified sulfide catalysts on their basis were synthesized, their physicochemical characteristics were determined, and their performance in the reactions of hydrodesulfurization (HDS) of dibenzothiophene (DBT) and hydrogenation of naphthalene was evaluated. Modification of the Mo-containing catalysts with vanadium by impregnation with a solution of mixed heteropoly acids was found to enhance their catalytic activity in the studied reactions, as well as to increase the selectivity for the direct hydrodesulfurization route of the DBT HDS reaction.