Photocatalysis　offers　a　green　and　promising　strategy　for　light-driven　pollutant　degradation　to　address　water　pollution.　Yet,　challenges　in　conversion　efficiency　and　cost-efficiency　propel　the　search　for　effective　metal-free　photocatalysts.　Here,　we　employ　a　ball　milling　technique　using　organic　solvent　molecules　to　enhance　the　exfoliation　of　g-C3N4　nanosheets.　Incorporating　tetrahydrofuran,　with　its　distinctive　five-membered　monooxygenase　ring　structure,　endows　exfoliated　CN　nanosheets　(TCN)　with　remarkable　electron-donating　capabilities,　expanding　specific　surface　area　and　active　sites,　essential　for　intricate　photocatalytic　reactions.　Comparative　assessments　unequivocally　establish　TCN＇s　superiority,　revealing　a　remarkable　3.6-fold　enhancement　in　RhB　dye　degradation　and　a　remarkable　99.7　%　removal　efficiency.　TCN　demonstrates　rapid,　complete　reduction　of　heavy　metal　ions　(Cr6+)　under　natural　sunlight　within　10　min　and　exhibits　a　significant　2.3-fold　antibiotic　degradation　enhancement　over　pristine　CN.　This　pioneering　work　unveils　the　mechanisms　behind　TCN＇s　superior　photocatalytic　performance,　offering　insights　into　designing　advanced　photocatalysts　for　crucial　water　purification　applications.　©　2023　Elsevier　B.V.