Hydrodeoxygenation　(HDO)　is　an　important　catalytic　route　for　upgrading　of　biomass　resources　to　biofuels.　The　cleavage　of　aryl　C-O　bond　is　the　key　step　to　remove　oxygen　atoms　from　biomass　molecules,　however,　which　usually　occurs　after　the　cleavage　of　alkyl　C-O　bond　in　thermodynamics　due　to　the　significant　higher　bond　energy　of　aryl　C-O　bond.　Herein,　we　report　a　series　of　Pt/α-MoC　catalysts　with　different　Pt　concentration　for　the　HDO　of　anisole,　a　biomass　molecule.　The　Pt/α-MoC　catalyst　exhibits　enhanced　HDO　catalytic　performance　in　terms　of　the　higher　turnover　rate　(150.2　h−1)　and　lower　apparent　activation　energy　(42.5–48.2　kJ·mol−1)　compared　with　primitive　α-MoC　catalyst.　By　temperature　programmed　surface　reaction　and　X-ray　absorption　spectrum,　the　status　of　Pt　in　the　Pt/α-MoC　catalyst　is　revealed　to　be　atomically　dispersed　on　α-MoC　when　the　Pt/Mo　ratio　is　lower　than　0.2　%.　The　singly　dispersed　PtMo　bimetallic　sites　serve　as　the　catalyst　for　HDO,　and　attribute　to　the　dissociation　of　aryl　C-O　bond　prior　to　that　of　alkyl　C-O　bond.　This　work　identifies　the　role　of　Pt　in　the　carbide　catalyst　for　HDO,　and　further　provides　new　insight　for　catalyst　design　towards　to　selective　C-O　bond　cleavage.　©　2022　Elsevier　B.V.