Current carbon capture technologies face a critical trade-off between CO2 absorption capacity and regeneration energy requirements. We present an approach to reduce the regeneration energy load using a thermally responsive pH regulator in aqueous carbonate solutions. By leveraging the temperature-dependent equilibrium constant of the regulator, our system achieves enhanced CO2 uptake at ambient conditions and enables low-temperature CO2 desorption (≤ 60 °C, 1 atm) through controlled pH swing. A continuous-flow reactor demonstrates the efficient concentration of diluted CO2 streams (1-5%) to high-purity products with low energy inputs (even solely with natural sunlight), remarkable stability (>240 hours), and attractive economics. This work represents a sustainable carbon capture technology that offers a pragmatic pathway for industrial-scale implementation while minimizing energy penalties associated with traditional CO2 capture processes.