Hydrodeoxygenation (HDO) of 5-hydroxymethylfurfural (HMF) was examined over well-defined and uniform, Pt-Ni, Pt-Zn and Pt-Cu alloyed nanocrystals (NCs) supported on carbon, at 33 bar and between 160 and 200 °C. Pt-Ni alloy catalysts were prepared in three different Pt:Ni ratios, Pt6Ni, Pt3Ni, and PtNi. While all of the Pt-Ni alloys were more selective for producing 2,5-dimethylfuran (DMF) than were Pt or Ni monometallic catalysts, the Pt3Ni catalyst was superior to the other compositions, exhibiting a yield of 98% due to its optimum surface composition. Similarly high yields were obtained on catalysts prepared from Pt2Zn and PtCu NCs. Possible reasons are given for why each of the Pt-alloy catalysts is highly selective