Carbon supported Pt-Ru nano-alloy with multiple reactive sites exhibits unprecedentedly efficient performance in acetone hydrogenation at room temperature. Catalytic properties can be controllably regulated and optimized via performing the specific annealing treatment for the catalyst. The essential correlation between the variations in catalyst's annealing conditions and the resultant variation in catalytic properties has been explored and discussed as a structure-function relationship. The combination of Pt and Ru sites exhibits enhanced catalytic activity compared with monometallic ones. Larger PtRu alloy particle size favors the rapid C=O hydrogenation and the improvement of catalytic selectivity to isopropanol. Isopropyl ether generation is related to the Pt defect sites on the surface, which can be blocked though the catalyst's oxidation treatment. The presence of surface metal-oxide species is beneficial to the performance enhancement, resulting from the synergetic behavior between metal-oxide sites and metallic sites on respectively activating the reactants. Moreover, 3-pentanone is used as a probe molecule to verify the structure-function relationship of catalytic low-temperature C=O hydrogenation on PtRu/C. (C) 2018 Elsevier Inc. All rights reserved.