Oxidation,　especially　selective　oxidation　by　a　heterogeneous　catalyst　with　molecular　oxygen,　is　a　core　technology　for　the　conversion　of　petrochemical　feedstock　to　commodity　chemicals　and　pharmaceuticals.　Existing　catalytic　approaches　for　efficient　aerobic　oxidation　normally　rely　on　the　engagement　of　organometallic　centers　or　transition-metal　nanoparticles.　In　light　of　the　necessity　to　develop　sustainable　production　methodologies,　multiple　approaches　for　the　metal-free　polymeric　carbon　nitride　(PCN)　photocatalytic　selective　oxidation　have　been　evaluated.　However,　the　insufficient　visible　light　optical　absorption,　poor　charge-carriers　separation　and　the　weak　driving　force　towards　oxidation　reaction　impart　a　serious　restriction　on　the　eciency　and　selectivity　of　the　organic　photosynthesis,　especially　under　extended　wavelength　solar　light　irradiation.　Here,　we　report　a　surface　engineering　photochemical　modification　method　to　fabricate　a　donor-acceptor　(D-A)　functional　carbon　nitride　photocatalyst　(ECN)　under　ambient　conditions.　The　well-developed　D-A　structure,　preserved　high　crystallinity　and　enlarged　π-conjugation　framework　of　the　hybrid　semiconductor-molecule　ECN　samples　favor　the　improvement　of　the　optical　absorption,　as　well　as　the　enhanced　separation　and　migration　of　the　photo-generated　charge　carriers.　As　a　result,　the　obtained　ECN　photocatalysts　exhibited　remarkable　enhancement　in　the　photocatalytic　aerobic　oxidation　of　alcohols,　even　under　an　extended　light　wavelength　of　620　nm　red-light　irradiation.　The　photocatalytic　aerobic　sulfides　and　sp3　C–H　oxidation　reactions　were　also　considerably　accelerated　over　ECN　and　may　serve　as　a　direct　approach　for　the　construction　of　value-added　sulfoxide　and　ketone　products.　©　2021　Elsevier　B.V.