This work reports the synthesis of mesoporous SBA-15 and Al-SBA-15-supported nickel phosphide nanocatalysts and the investigation of their bifunctional property in catalyzing the one-pot conversion of cellobiose to sorbitol. The SBA-15-supported nickel phosphide nanocatalysts were prepared with three different wt.% ratios of Ni/P: 10:2, 10:3, and 10:4. The Al-SBA-15 support was also used, where the wt.% ratio of Ni/P of 10:4 was applied for the preparation. The prepared nanocatalysts were characterized by XRD, N-2 adsorption-desorption, SEM, TEM, and NH3-TPD, confirming the successful incorporation of nickel phosphide nanoparticles on (Al-)SBA-15 and the preservation of the hexagonal structure of the support after the modification processes. Notably, the characterization results also indicate that each catalyst contained different crystalline phases of nickel phosphide. The synthesized nanocatalysts were tested for their catalytic performance in the hydrolytic hydrogenation of cellobiose to produce sorbitol under the following conditions: 150 degrees C, 3 h, 4 MPa of H-2. Three major products including glucose, sorbitol, and mannitol were obtained by all catalytic reactions. The proportions of these products, however, differed by the presence of different phases of nickel phosphide in each catalyst. The effect of reaction temperature and that of support materials on the catalytic performance are also studied.