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Achieving CO oxidation at room temperature is significant for gas purification but still challenging nowadays. Pt promoted by 3d transition metals (TMs) is a promising candidate for this reaction, but TMs are prone to be deeply oxidized in an oxygen-rich atmosphere, leading to low activity. Herein we report a unique structure design of graphene-isolated Pt from CoNi nanoparticles (PtǀCoNi) for efficiently catalytic CO oxidation in an oxygen-rich atmosphere. CoNi alloy is protected by ultrathin graphene shell from oxidation and therefore modulates the electronic property of Pt-graphene interface via electron penetration effect. This catalyst can achieve near 100% CO conversion at room temperature, while there are limited conversions over Pt/C and Pt/CoNiOx catalysts. Experiments and theoretical calculations indicate that CO will saturate Pt sites, but O2 can adsorb at the Pt-graphene interface without competing with CO, which facilitate the O2 activation and the subsequent surface reaction. This graphene-isolated system is distinct from the classical metal-metal oxide interface for catalysis, and it provides a new thought for the design of heterogeneous catalysts., Achieving CO oxidation at room temperature is significant for gas purification but remains challenging to perform. Here, the authors report design of graphene-isolated Pt from cobalt-nickel nanoparticles for efficiently catalytic CO oxidation in an oxygen-rich atmosphere.