A strategy of tuning azole-based ionic liquids for reversible CO2 capture from ambient air was reported. Through tuning the basicity of anion as well as the type of cation, an ideal azole-based ionic liquid with both high CO2 capacity and excellent stability was synthesized, which exhibited a highest single-component isotherm uptake of 2.17 mmol/g at the atmospheric CO2 concentration of 0.4 mbar at 30 oC, even in the presence of water. The bound CO2 can be released by relatively mild heating of the IL-CO2 at 80 oC, which mike it promising for energy-efficient CO2 desorption and sorbent regeneration, leading to excellent reversibility. To the best of our knowledge, these azole-based ionic liquids are superior to other adsorbent materials for direct air capture due to their dual-tunable properties and high CO2 capture efficiency, offering a new prospect for efficient and reversible direct air capture technologies.