Lattice　oxygen　(OL)　redox　chemistry　is　a　key　to　alleviating　the　energy　and　environmental　crisis,　but　it　faces　challenges　in　activating　the　OL　while　ensuring　structural　stability.　We　disclosed　herein　that　engineering　a　heterogeneous　interface　between　ultrathin　oxide　and　amorphous　carbon　can　attain　the　durable　OL　redox　chemistry　without　introducing　catalytically　impure　sites.　To　this　end,　we　proposed　a　green　strategy　to　grow　∼3.9　nm-thickness　wrinkled　δ-MnO2　nanosheets　that　are　rich　in　defects　and　are　vertically　aligned　on　amorphous　carbon　spheres.　Experiments　and　calculations　reveal　that　the　electrons　can　easily　migrate　from　the　amorphous　carbon　to　MnO2　at　the　δ-MnO2@C　heterointerface.　The　heterogeneous　interfaces　can　not　only　regulate　the　Mn-O　bond　and　create　oxygen　defects　in　δ-MnO2　but　also　introduce　lattice　oxygen　with　varying　reactivities.　Specifically,　the　δ-MnO2@C　structure　carries　more　activated　lattice　oxygen　that　contributes　to　the　enhanced　activity　on　catalytic　oxidation　of　bioderived　5-hydroxymethylfurfural　(HMF)　to　2,5-furandicarboxylic　acid　(FDCA),　with　a　high　FDCA　formation　rate　of　1759　μmol　gcat-1　h-1　and　a　high　selectivity　of　95%.　The　heterogeneous　interface　of　MnO2@C　also　brings　inert　lattice　oxygen,　so　that　it　manifests　high　structural　stability　during　the　oxidation　reactions.　This　work　deepens　the　fundamental　understandings　in　the　engineering　of　lattice　oxygen　for　durable　lattice　oxygen　redox　chemistry　and　showcases　an　effective　interface　technique　in　creating　advanced　catalysts　for　clean　sustainable　energy.　©　2024　American　Chemical　Society.