Direct　selective　oxidation　of　methane　(DSOM)　to　highvalue-addedoxygenates　under　mild　conditions　is　attracting　considerable　interest.Although　state-of-the-art　supported　metal　catalysts　can　improve　methaneconversion,　it　is　still　challenging　to　avoid　the　deep　oxidation　ofoxygenates.　Here,　we　develop　a　highly　efficient　metal-organicframeworks　(MOFs)-supported　single-atom　Ru　catalyst　(Ru-1/UiO-66)　for　the　DSOM　reaction　using　H2O2　asan　oxidant.　It　endows　nearly　100%　selectivity　and　an　excellent　turnoverfrequency　of　185.4　h(-1)　for　the　production　of　oxygenates.The　yield　of　oxygenates　is　an　order　of　magnitude　higher　than　thaton　UiO-66　alone　and　several　times　higher　than　that　on　supported　Runanoparticles　or　other　conventional　Ru-1　catalysts,　whichshow　severe　CO2　formation.　Detailed　characterizations　anddensity　functional　theory　calculations　reveal　a　synergistic　effectbetween　the　electron-deficient　Ru-1　site　and　the　electron-richZr-oxo　nodes　of　UiO-66　on　Ru-1/UiO-66.　The　Ru-1　site　is　responsible　for　the　activation　of　CH4　via　theresulting　Ru-1=O*　species,　while　the　Zr-oxo　nodesundertake　the　formation　of　oxygenic　radical　species　to　produce　oxygenates.In　particular,　the　Zr-oxo　nodes　retrofitted　by　Ru-1　canprune　the　excess　H2O2　to　inactive　O-2　more　than　(OH)-O-center　dot　species,　helping　to　suppress　theover-oxidation　of　oxygenates.