A　novel　pulsed　laser-assisted　modification　was　firstly　employed　to　tailor　the　doping　configuration　of　heteroatoms　into　graphitic　carbon　nitride　(g-C3N4).　Compared　with　the　traditional　thermal　treatment　to　form　single　boron　doping　configurations　(BCN-A),　the　laser　modification　could　in　situ　incorporate　boron　dopants　with　two　distinct　configurations　(corner　(B-(N)3)　and　bay　(H-B-(N)2)　motifs)　(BCN-L).　Experimental　characterizations　and　theory　simulations　reveal　that　the　cyano　group　induces　defect　levels　near　the　valence　band　(VB)　maximum,　while　its　incorporation　with　the　H-B-(N)2　motifs　results　in　the　relocation　of　these　defect　levels　to　the　vicinity　of　conduction　band　(CB)　minimum.　This　modification　effectively　tunes　the　band　structure　of　the　g-C3N4,　enhancing　charge　separation　efficiency　and　extending　the　range　of　light　absorption.　Moreover,　the　B-(N)3　motifs　at　the　corners　significantly　increased　surface　charge　polarization,　which　boosted　the　adsorption　of　oxygen　molecules　and　promoted　electron　transfer　at　the　catalyst/O2　interface.　Density　functional　theory　simulation　further　revealed　that　the　strong　interactions　between　boron　and　oxygen　atoms　could　boost　oxygen　adsorption　and　promote　the　formation　of　intermediate　•O2−,　which　represents　the　initial　step　in　this　reaction　mechanism.　With　these　beneficial　characteristics,　the　photocatalytic　H2O2　production　rate　of　the　modified　g-C3N4　reached　994.1　μmol　g−1h−1,　which　indicates　a　significant　increase　from　the　239.6　μmol　−1h−1　of　the　pristine　g-C3N4.　Furthermore,　the　optimal　BCN-L　demonstrated　significant　photo-corrosion　resistance,　which　maintained　high　catalytic　activity　for　10　h　of　continuous　operation　without　noticeable　degradation,　achieving　a　total　H2O2　yield　of　10.2　mmol　g−1.　©　2025　Elsevier　B.V.