Highly dispersed Pt-Co bimetallic catalysts were deposited on multi-walled carbon nanotubes (MWCNTs) by atomic layer deposition. High-resolution TEM and TPR analysis verified the formation of Pt-Co bimetallic particles. Catalysts were applied for hydrogenolysis of 5-hydroxymethyfurfural (HMF) to 2,5-dimethyfuran (DMF). High yield of DMF (> 90%) was achieved in hydrogenolysis of HMF over the optimized Pt-Co/MWCNTs catalyst after 8 hr of reaction time under 10 bar H2 at 160 ºC. Through a series of experiments and comparison, the synergistic effect among Pt, Co, and MWCNTs was investigated. The results revealed that the synergistic effect between Pt-Co and MWCNTs played an important role in the improvement of selectivity to DMF for Pt-Co/MWCNTs bimetallic catalysts. In addition, steric hindrance appeared when the Co loading in Pt-Co/MWCNTs was high and it affected the activity of Pt-Co bimetallic catalysts. However, the moderate activity can inhibit the production of byprodct and thereby improve the yield of DMF.