Nitrogen-doped　carbon　materials　as　metal-free　catalysts　have　attracted　considerable　attention　in　selective　oxidation　of　benzyl　alcohol.　However,　the　real　active　sites　are　still　ambiguous　due　to　complexities　of　surface　functional　groups　and　nitrogen　species.　Herein,　a　series　of　nitrogen-doped　nanosheets　with　different　N　species　content　are　simply　fabricated,　which　exhibits　excellent　catalytic　activity　with　82–93　%　conversion　and　89–99　%　selectivity　in　selective　oxidation　of　benzyl　alcohol　into　benzaldehyde.　Moreover,　it　is　demonstrated　that　the　conversion　of　benzyl　alcohol　mainly　depends　on　the　hydroxyl　functional　groups,　while　both　graphitic　and　pyridinic　nitrogen　are　key　factors　to　determine　the　selectivity　of　benzaldehyde.　The　present　work　demonstrates　the　structure-activity　relationships　between　the　catalytic　performance　for　catalytic　oxidation　of　benzyl　alcohol　and　the　surface　functional　groups　of　catalysts,　paving　the　way　for　development　of　highly　efficient　nanocarbon　catalysts.　©　2022　Elsevier　B.V.