Photocatalytic　conversion　of　CO2　into　value-added　chemical　fuels　is　a　promising　approach　to　address　the　depletion　of　fossil　energy　and　environment-related　concerns.　Tailor-making　the　electronic　properties　and　band　structures　of　photocatalysts　is　pivotal　to　improve　their　efficiency　and　selectivity　in　photocatalytic　CO2　reduction.　Herein,　a　covalent　triazine-based　framework　was　developed　containing　electron-donor　triphenylamine　and　electron-acceptor　triazine　components　(DA-CTF).　The　engineered　π-conjugated　electron　donor–acceptor　dyads　in　DA-CTF　not　only　optimized　the　optical　bandgap　but　also　contributed　to　visible-light　harvesting　and　migration　of　photoexcited　charge　carriers.　The　activity　of　photocatalytic　CO2　reduction　under　visible　light　was　significantly　improved　compared　with　that　of　traditional　g-C3N4　and　reported　covalent　triazine-based　frameworks.　This　study　provides　molecular-level　insights　into　the　mechanism　of　photocatalytic　CO2　reduction.　©　2019　Wiley-VCH　Verlag　GmbH　&　Co.　KGaA,　Weinheim