Conventional desalination membrane technologies, although offer portable drinking water, are still energy-intensive processes. This paper proposes a potentially new approach for performing water desalination and purification by utilizing the reversible interaction of carbon dioxide (CO2) with nucleophilic amines-reminiscent of the Solvay process. Based on our model studies with small molecules, CO2-responsive amphiphilic insoluble diamines were prepared, characterized, and applied in the formation of soda and ammonium chloride upon exposure to ambient CO2 (1atm), thus removing chloride ions from model and real seawater. This ion-exchange process and separation of chloride from the aqueous phase are spontaneous in the presence of CO2 without the need for external energy sources. We demonstrate a flow system to envisage energy-efficient CO2-mediated desalination and simultaneous carbon capture and sequestration.