Currently, the base-free aerobic oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA) is attracting intense interest due to its prospects for the green, sustainable, and promising production of biomass-based aromatic polymers. Herein, we have developed a new Pt catalyst supported on nitrogen-doped-carbon-decorated CeO (NC-CeO ) for the aerobic oxidation of HMF in water without the addition of any homogeneous base. It was demonstrated that the small-sized Pt particles could be well dispersed on the surface of the hybrid NC-CeO support, and the activity of the supported Pt catalyst depended strongly on the surface structure and properties of the catalysts. The as-fabricated Pt/NC-CeO catalyst, with abundant surface defects, enhanced basicity, and favorable electron-deficient metallic Pt species, enabled an almost 100 % yield of FDCA in water with molecular oxygen (0.4 MPa) at 110 °C for 8 h without the addition of any homogeneous base, which is indicative of exceptional catalytic performance. Furthermore, this Pt/NC-CeO catalyst also showed good stability and reusability owing to strong metal-support interactions. An understanding of the role of surface structural defects and basicity of the hybrid NC-CeO support provides a basis for the rational design of high-performance and stable supported metal catalysts with practical applications in various transformations of biomass-derived compounds.