The　O3-type　Li-rich　layered　oxides　(LLOs)　are　approaching　industrial　applications　as　high-energy　cathode　materials　for　Li-ion　batteries　(LIBs),　however,　they　suffer　from　rapid　performance　decay　associated　with　oxygen　activities.　The　interplay　between　surface　and　bulk　transformations　in　LLOs,　especially　the　electrochemical　behaviors　of　oxygen　anions,　remains　elusive.　Here,　by　regulating　the　surface　of　an　O3-type　LLO　(Li1.13Mn0.517Ni0.256Co0.097O2)　using　an　all-fluorinated　electrolyte,　an　enhanced　capacity　retention　from　57.4%　to　85.3%　and　a　suppressed　voltage　decay　from　1.34　mV　cycle(-1)　to　0.58　mV　cycle(-1)　within　300　cycles　are　realized.　The　performance　enhancement　is　attributed　to　the　thin,　uniform,　robust,　and　compact　F-rich　cathode-electrolyte　interphase　(CEI),　which　suppresses　various　types　of　oxygen-related　surface　degradation　and,　more　importantly,　stabilizes　the　bulk　oxygen　reactions.　Through　the　combined　experimental　and　theoretical　studies,　this　work　directly　reveals　the　intriguing　association　between　the　surface　and　bulk　oxygen　activities　and　demonstrates　that　optimizing　the　interphase　is　an　effective　approach　for　improving　the　stability　of　high-energy　battery　cathodes　involving　oxygen　redox　reactions.