The hydrodeoxygenation (HDO) of furfural to 2-methylfuran (MF) was investigated in a continuous flow reactor over carbon-supported, PtCo3 nano-crystals (NCs) and NiFe bimetallic catalysts, along with their monometallic counterparts, at 1 and 33 bar, respectively. At 1 bar, the decarbonylation reaction to furan was a major nonselective pathway on both PVC and Ni/C; but this pathway was almost eliminated on the bimetallic catalysts. At 33 bar, decarbonylation is not observed on any of the catalysts and the major non-selective reaction pathway on both Ni and Pt catalysts is the over-hydrogenation of MF. Catalysts based on both PtCo3 NCs and NiFe bimetallics also suppress the over-hydrogenation reactions and are able to achieve significantly better MF yields under these conditions as well. The implications of these results for understanding HDO reactions on bimetallic catalysts are discussed.