Seeking　highly-efficient,　non-pollutant,　and　chemically　robust　photocatalysts　for　visible-light-driven　ammonia　production　still　remained　challenging,　especially　in　pure　water.　The　key　bottle-necks　closely　correlate　to　the　nitrogen　activation,　water　oxidization,　and　hydrogen　evolution　reaction　(HER)　processes.　In　this　study,　a　novel　Bi　decorated　imine-linked　COF-TaTp　(Bi/COF-TaTp)　through　N-Bi-O　coordination　is　reasonably　designed　to　achieve　a　boosting　solar-to-ammonia　conversion　of　61　mu　mol(-1)　g(-1)　h(-1)　in　the　sacrificial-free　system.　On　basis　of　serial　characterizations　and　DFT　calculations,　the　incorporated　Bi　is　conducive　to　the　acceleration　of　charge　carriers　transfer　and　N-2　activation　through　the　donation　and　back-donation　mode.　The　N-2　adsorption　energy　of　5%　Bi/COF-TaTp　is　calculated　to　be　-0.19　eV　in　comparison　with　-0.09　eV　of　the　pure　COF-TaTp　and　the　electron　exchange　between　N-2　and　the　modified　catalyst　is　much　more　intensive.　Moreover,　the　accompanied　hydrogen　production　process　is　effectively　inhibited　by　Bi　modification,　demonstrated　by　the　higher　energy　barrier　for　HER　over　Bi/COF-TaTp　(2.62　eV)　than　the　pure　COF-TaTp　(2.31　eV)　when　using　H　binding　free　energy　(Delta　G(H*))　as　a　descriptor.　This　work　supplies　novel　insights　for　the　design　of　photocatalysts　for　N-2　reduction　and　intensifies　the　understanding　of　N-2　adsorption　and　activation　over　covalent　organic　frameworks-based　materials.