Transition metal phosphide nanoparticles supported on silica were used as catalysts to investigate the hydrodeoxygenation of methyl laurate (used as a model compound for vegetable oils). Ni2P, Ni1Mo1P, and Ni1.6Mo0.4P were synthesized using a molecular precursor route. The nanoparticles were added to the silica support without any changes in their structure or particle size. As a reference and for comparison, MoP/SiO2 was also prepared by the phosphite method. The prepared catalysts were characterized by X‐ray diffraction, X‐ray photoelectron spectroscopy, transmission electron microscopy, and chemical analysis. A higher conversion is reached with the MoP/SiO2 monometallic catalyst, close to that with Ni1Mo1P/SiO2. However, this observation is misleading because the differences in dispersion obscure the result that the intrinsic activity (turnover frequency) of the bimetallic catalyst, prepared by a molecular precursor route, is significantly higher than that of the monometallic catalyst, prepared by the phosphite route, revealing a synergistic effect on the catalytic activity due to the formation of the bimetallic phosphide.