This paper demonstrates a one-pot approach to produce highly dispersed dendritic palladium-platinum bimetallic nanoparticles (NPs) with small particle size, tunable composition and high catalytic activity. Herein, the PdPt bimetallic NPs have been obtained using bayberry tannin (BT) as both the reducing agent and surfactant. Additionally, the PdPt bimetallic NPs with different Pd/Pt atomic ratios can be prepared by just varying the amounts of the Pd and Pt precursors. Most importantly, the as-prepared Pd 52 Pt 48 catalyst exhibits the optimal catalytic activities compared with the other compositional PdPt NPs (Pd 82 Pt 18 , Pd 69 Pt 31 , and Pd 36 Pt 64 ) and commercial Pt/C (20 wt.%) catalyst for the methanol oxidation reaction (MOR). Meanwhile, Pd 52 Pt 48 also shows better CO tolerance, which can be attributed to the unique dendritic structure and the synergistic effect between Pd and Pt. With evident advantages of the facile preparation and enhanced catalytic performance, it holds great promise as a high-performance catalyst for electrochemical energy conversion.