Bimetallic　catalyst　is　a　major　group　of　the　heterogeneous　catalysts　which　has　been　widely　investigated　for　many　important　catalytic　processes　such　as　biomass　upgrading.　The　synergistic　effect　between　two　transition　metal　of　bimetallic　catalyst　plays　a　vital　role　to　promote　catalytic　performance.　In　this　work,　the　Pd-Mo　bimetallic　catalysts　were　investigated　for　the　hydrodeoxygenation　(HDO)　of　a　biomass-derived　molecule,　anisole.　The　synergistic　effect　was　confirmed　in　the　Pd-Mo　bimetallic　catalyst.　The　correlated　structure　features　of　the　Pd　and　Mo　sites　during　catalysis　have　been　revealed　to　understand　the　synergistic　effect.　It　is　found　that　the　Mo　species　are　partially　reduced　and　cover　around　Pd　nanoparticles.　As　the　results,　the　crystalline　status,　redox　properties,　electron　state　and　adsorption　behaviors　of　Pd　species　are　greatly　influenced　by　Mo　species.　Moreover,　the　formation　of　Pd-Mo　bond　is　directly　observed　by　in-situ　X-ray　absorption　spectrum.　This　work　brings　new　insights　to　understand　the　structure　origination　for　the　synergistic　effect　in　bimetallic　catalyst.　©　2022