Abstract Concerns over global climate change have led to strong research emphasis worldwide on reducing the emission of greenhouse gases like CO2. One avenue for carbon emission reduction is using CO2 capture and storage from industrial sources. Having low toxicity and low vapor pressure and being resistant to oxidation, natural amino acids could be a better choice over current carbon capture materials. In this study, we pioneered a unique phase change amino acid salt solvent concept in which amino acid salt solution was turned into a CO2-rich phase and a CO2-lean phase upon simple bubbling with CO2 and most importantly, this solution captured the most CO2 (∼90%) in the CO2-rich phase. Bicarbonate was found to be dominant in the CO2-rich phase, which had a high CO2 loading capacity and good regenerability and cycling properties. Such a phase change amino acid salt solvent may provide unique solutions for industries to reduce CO2 and other harmful emissions.