Despite　the　pivotal　role　of　molecular　oxygen　(O-2)　activation　in　artificial　photosynthesis,　the　activation　efficiency　is　often　restricted　by　sluggish　exciton　dissociation　and　charge　transfer　kinetics　within　polymer　photocatalysts.　Herein,　we　propose　two　tetrathiafulvalene　(TTF)-based　imine-linked　covalent　organic　frameworks　(COFs)　with　tailored　donor-acceptor　(D-A)　structures,　TTF-PDI-COF　and　TTF-TFPP-COF,　to　promote　O-2　activation.　Because　of　enhanced　electron　push-pull　interactions　that　facilitated　charge　separation　and　transfer　behavior,　TTF-PDI-COF　exhibited　superior　photocatalytic　activity　in　electron-induced　O-2　activation　reactions　over　TTF-TFPP-COF　under　visible　light　irradiation,　including　the　photosynthesis　of　(E)-3-amino-2-thiocyano-alpha,beta-unsaturated　compounds　and　H2O2.　These　findings　highlight　the　significant　potential　of　the　rational　design　of　COFs　with　D-A　configurations　as　suitable　candidates　for　advanced　photocatalytic　applications.