This　work　demonstrates　the　molecular　engineering　of　active　sites　on　a　graphene　scaffold.　It　was　found　that　the　N-doped　graphene　nanosheets　prepared　by　a　high-temperature　nitridation　procedure　represent　a　novel　chemical　function　of　efficiently　catalyzing　aerobic　alcohol　oxidation.　Among　three　types　of　nitrogen　species　doped　into　the　graphene　lattice-pyridinic　N,　pyrrolic　N,　and　graphitic　N-　the　graphitic　sp(2)　N　species　were　established　to　be　catalytically　active　centers　for　the　aerobic　oxidation　reaction　based　on　good　linear　correlation　with　the　activity　results.　Kinetic　analysis　showed　that　the　N-doped　graphene-catalyzed　aerobic　alcohol　oxidation　proceeds　via　a　Langmuir-Hinshelwood　pathway　and　has　moderate　activation　energy　(56.1　+/-　3.5　kJ.mol(-1)　for　the　benzyl　alcohol　oxidation)　close　to　that　(51.4　kJ.mol(-1))　proceeding　on　the　catalyst　Ru/Al2O3　reported　in　literature.　An　mechanism　was　proposed　to　be　different　remarkably　from　that　occurring　on　the　noble　metal　catalyst.　The　possible　formation　of　a　sp(2)　N-O-2　adduct　transition　state,　which　can　oxidize　alcohols　directly　to　aldehydes　without　any　byproduct,　including　H2O2　and　carboxylic　acids,　may　be　a　key　element　step.　Our　results　advance　graphene　chemistry　and　open　a　window　to　study　the　graphitic　sp(2)　nitrogen　catalysis.