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[Display omitted] Constructing donor–acceptor structures in polymeric carbon nitride (CN) provides an attractive pathway for facilitating charge carrier separation in photocatalytic reactions. However, achieving the implantation of donor or acceptor moieties at molecule level precision remains challenging. Here we develop a three-dimensional (3D) porous thiophene implanted carbon nitride (TCN) with donor–acceptor structure via a supramolecular assembly strategy. The specific-designed triazine derivatives with similar hydrogen bonding sites allow for the uniform introduction of thiophene groups at molecule level precision during the supramolecular assemble stage. The electron-donating thiophene groups in TCN can continuously tune electronic band structure, expand visible light absorption range, and promote charge carriers' separation. The optimized properties enable TCN-3 an outstanding H 2 evolution rate of 5620 μmol h−1 g−1, greatly exceeding bulk CN (95 μmol h−1 g−1). Briefly, our work may offer opportunities to prepare highly active photocatalysts with molecule level precise donor–acceptor structure. [ABSTRACT FROM AUTHOR]