Selective hydrogenation and hydrogenolysis of 5‐hydroxymethylfurfural (HMF) to 2,5‐bis(hydroxymethyl)furan (BHMF) and 2,5dimethylfuran (DMF) were explored by regulating the nanosized Pt on Co/Al2O3 catalysts. Characterization results revealed that the catalyst acidity was influenced by adjusting the Co/Pt composition, while the addition of more Pt loading on Co/Al2O3 catalysts resulted in a facilitation of H2 reduction process. Lower size of catalyst particles was obtained for the Co‐Pt system in comparison to the monometallic Co/Al2O3 catalyst. Additionally, the structural characterizations by XRD, XANES, and XPS established the co‐existences between metallic Pt0/Co0 and oxophilic PtO2/CoOx, acting as the active components for the reactions. Operated under a full HMF conversion, the Co1Pt0.050Al catalyst with high Pt loading gave >99.9% BHMF selectivity at 40 oC; whereas, an 86.7% of DMF selectivity was noticeable over low Pt loading of the Co1Pt0.013Al catalyst at 160 oC. This investigation evidenced that the selective production of BHMF or DMF towards hydro‐conversion of HMF was relied on the amount of Pt contents on Co/Al2O3 catalyst, in which the metal sizes and acidity had meaningful effects on the hydrogenation and hydrogenolysis processes.