Poor electrocatalytic activity and carbon monoxide (CO) poisoning of the anode in Pt-based catalysts are still two major challenges facing direct methanol fuel cells. Herein, we demonstrate a highly active and stable Pt nanoparticle/Mo 2 C nanotube catalyst for methanol electro-oxidation. Pt nanoparticles were deposited on Mo 2 C nanotubes using a controllable atomic layer deposition (ALD) technique. This catalyst showed much higher catalytic activity for methanol oxidation and superior CO tolerance, when compared with those of the conventional Pt/C and PtRu/C catalysts. The experimental evidence from X-ray absorption near-edge structure spectroscopy and scanning transmission X-ray microscopy clearly support a strong chemical interaction between the Pt nanoparticles and Mo 2 C nanotubes. Our studies show that the existence of Mo 2 C not only minimizes the required Pt usage but also significantly enhances CO tolerance and thus improves their durability. These results provide a promising strategy for the design of highly active next-generation catalysts.