Biomimetic photosynthesis, which leverages nanomaterials with light-responsive capabilities, represents an innovative approach for replicating natural photosynthetic processes for green and sustainable energy conversion. In this study, a covalent-organic framework (COF)-based artificial photosynthesis system is realized through the co-assembly of adenosine triphosphate (ATP) synthase and a light-responsive proton generator onto an imine-based COF, RT-COF-1. This system demonstrates an ATP production rate of 0.64 µmol ATP per mg protein within 90 s of light exposure and, for the first time, exhibites regenerative ATP production through multiple light on/off cycles. Furthermore, the ATP generated by the system facilitates the biocoupling of monosaccharides into disaccharides, confirming the hybrid system's capability to convert solar energy into chemical energy in the form of organic molecules. This approach shows significant potential for renewable bioenergy generation, offering precise and reliable control over biochemical processes through artificial photosynthesis.