Materials for CO capture have been extensively exploited for climate governance and gas separation. However, their regeneration is facing the problems of high energy cost and secondary CO contamination. Herein, a reversed photosynthesis-like process is proposed, in which CO is absorbed in darkness while being released under light illumination. The process is likely supplementary to natural photosynthesis of plants, in which, on the contrary, CO is released during the night. Remarkably, the material used here is able to capture 9.6 wt.% CO according to its active component. Repeatable CO capture at room temperature and release under light irradiation ensures its convenient and cost-effective regeneration. Furthermore, CO released from the system is successfully converted into a stable compound in tandem with specific catalysts.