AbstractCapture and storage of fossil carbon emitted to the atmosphere from anthropogenic sources has been identified as a key technology for keeping human‐induced global warming below 2°C. Available technologies have not achieved widespread impact due to costs related to increased energy consumption and expensive, large process equipment. Here, we show how molten inorganic halide salt‐based mixtures containing CaO may be utilized for selective capture and subsequent controlled release of carbon dioxide from diluted flue gases. Highly efficient absorption is demonstrated in a fluoride‐based liquid, absorbing close to 100% of the CO2 from a simulated flue gas with an absorbing column height of only 10 cm. Greater than 90% carbonation with >80% regeneration to CaO was recorded. Excellent cyclability has been achieved with a chloride‐based liquid with 60% carbonation and 100% regeneration to CaO during four cycles. The high efficiencies may enable extraction of CO2 from highly diluted gas mixtures.