In this work, we have devised an efficient strategy for photochemical modulation of molecular photoswitches to facilitate carbon capture (Figure ). This approach draws inspiration from our lab's extensive work on electrochemical modulation of redox-active materials. In electrochemical modulation, the redox-active material is activated through electrochemical reduction. The resulting electron-rich state of the material is sufficiently basic or nucleophilic to capture CO2 from diluted sources. Subsequently, the CO2-saturated solution undergoes electrochemical oxidation to regenerate the resting state of the redox-active material, releasing concentrated CO2. This cyclic process effectively separates and concentrates CO2 from the diluted source.