Direct　photocatalytic　water　splitting　is　an　attractive　strategy　for　clean　energy,　in　which,　organic　photocatalytic　systems　with　broad　light-harvesting　region　and　efficient　charge　separation　are　highly　desired　and　still　challenging.　In　this　paper,　three　multi-branched　organic　dyes　were　designed　and　synthesized　with　dipolar,　V-shaped,　and　octupolar　geometries,　respectively.　The　multiple　intramolecular　charge　transfer　processes　by　electronic　pull-push　effect　along　the　branches　can　provide　more　channels　for　light-harvesting　and　carrier　transporting.　Also,　the　interactions　with　polymeric　carbon　nitride　(PCN)　can　be　optimized　by　multiple　anchoring　units　and　defect　filling　effect,　resulting　in　the　gradually　enhanced　photocatalytic　hydrogen　evolution　performance　with　the　increased　number　of　branches.　Accordingly,　the　highest　one　of　996.9　mu　mol　h(-1)　was　achieved,　which　is　over　40-folders　that　of　PCN/Pt　(24.8　mu　mol　h(-1))　under　the　same　conditions.　It　provides　an　efficient　strategy　for　molecular　design　of　organic　dyes　as　photocatalyst,　promoting　development　of　PHE　system　from　the　molecular　level.