The direct conversion of untreated microcrystalline cellulose into C2-C3 alcohols, through a one-pot process promoted by the heterogeneous bimetallic Pd/Fe3O4 catalyst, is presented. The process is selfsustainable without the addition of external molecular hydrogen or acid/basic promoters and is mainly selective toward ethanol. At 240 °C, a complete cellulose conversion was reached after 12 h with an ethanol molar selectivity of 51% among liquid products. The synergistic effect played by water (which aids in the chemical pretreatment means of cellulose through the hydrolysis process) and the Pd/Fe3O4 catalyst (which catalyzes the hydrogenolysis reaction driving the pattern of obtained products) is elucidated.