In　this　work,　a　synergistic　strategy　integrated　elemental　doping　and　defect　engineering　has　been　developed　to　modulate　the　electronic　and　bandgap　structure　of　g-C3N4　by　controlling　its　conjugated　aromatic　system.　Experimental　analysis　and　theoretical　calculations　conrm　that　the　generation　of　imbalanced　spatial　distributions　of　charge　carriers　not　only　greatly　increases　the　π-electron　availability,　but　also　decreases　the　energy　barrier　for　hydrogen　adsorption　due　to　the　synergistic　effect　of　the　high　valence　electron　of　the　W　dopant　and　the　decreased　electronegativity　by　two-coordinated　nitrogen　defects,　which　strengthens　the　charge　transfer　efficiency　and　favors　the　light　capturing　capability.　The　combined　benets　of　the　electronic,　optical　and　textural　modification　lead　to　a　signicant　improvement　of　photocatalytic　activity　of　3.3　mmol　h−1　g−1　for　hydrogen　evolution　under　λ　≥　400　nm　light　irradiation,　about　twentyfold　enhancement　than　that　of　pristine　g-C3N4.　Such　proposed　synergistic　strategy　provides　a　promising　route　to　promote　the　performance　of　g-C3N4　for　potential　applications　in　solar　energy　conversion.　©　2020　Hydrogen　Energy　Publications　LLC