Aerobic　oxidation　of　5-hydroxymethylfurfural　(HMF)　to　2,5-furandicarboxylic　acid　(FDCA)　offers　an　appealing　way　to　transform　the　biomass　feedstock　into　chemical　commodities　but　suffers　from　low　efficiency　and　selectivity　due　to　the　formation　of　5-formyl-2-furancarboxylic　acid　(FFCA)　byproduct.　Herein,　we　demonstrated　that　an　amorphous　MnO2　(amor-MnO2)　nanostructure　having　a　disordered　lattice　structure　can　carry　OL　of　high　reactivity　for　catalyzing　the　aerobic　oxidation　of　HMF　to　prepare　FDCA　efficiently　and　selectively.　The　FDCA　formation　rate　of　amor-MnO2　reaches　up　to　1307　μmolFDCA　gcat-1　h-1,　about　8.2　times　that　of　crystalline　MnO2　(cry-MnO2)　(160　μmolFDCA　gcat-1　h-1)　and　surpassing　many　other　state-of-the-art　Mn-based　catalysts.　Kinetic　studies　reveal　that　the　amor-MnO2　nanostructure　can　efficiently　convert　the　low-concentration　FFCA　intermediate　into　FDCA,　which　helps　tackle　the　rate-determining　step　in　the　HMF　→　FFCA　→　FDCA　oxidation　process.　Density　functional　theory　calculations　and　experimental　measurements　demonstrate　that　amor-MnO2　delivers　superior　lattice　oxygen　(OL)　activity　and　stronger　O2　adsorption　capability　when　compared　with　the　crystalline　counterpart.　The　findings　showcase　the　use　of　amorphous　materials　as　advanced　catalysts　for　achieving　sustainable　chemistry　industry.　©　2022　American　Chemical　Society.