The　development　of　donor–acceptor　(D-A)　covalent–organic　frameworks　(COFs)　has　emerged　as　a　promising　strategy　for　enhancing　photocatalytic　performance.　Although　most　studies　have　concentrated　on　2D　COFs,　research　into　their　3D　counterparts　remains　limited.　In　this　study,　we　rationally　designed　and　synthesized　a　carbazoyl　dicyanobenzene　derivative　(TBFCC)　as　an　intrinsic　D-A　building　block.　By　selecting　TAPA,　TAPB,　and　TAPT　as　the　donor,　acceptor-π,　and　acceptor　donors,　respectively,　we　synthesized　three　distinct　D-A-extended　COF　materials:　D-D-A,　A-π-D-A,　and　A-D-A.　Among　these,　3D-TAPT-COF,　featuring　an　A-D-A　structure,　exhibited　the　highest　hydrogen　evolution　rate　of　31.3 mmol g−1 h−1,　surpassing　most　previously　reported　3D　COF-based　photocatalysts.　This　superior　performance　is　attributed　to　its　A-D-A　configuration,　which　provides　multiple　charge　transfer　pathways　in　3D　space,　overcoming　the　electron　transport　limitations　inherent　in　2D　COFs.　Consequently,　this　feature　facilitates　efficient　separation　of　photogenerated　charges　within　the　framework　and　reduces　carrier　recombination,　thereby　optimizing　photocatalytic　efficiency.　©　2025　Wiley-VCH　GmbH.