Abstract Ionic liquids (ILs) have been used for carbon dioxide (CO2) capture, however, which have never been used as catalysts to accelerate CO2 capture. The record is broken by a uniquely designed IL, [EMmim][NTf2]. The IL can universally catalyze both CO2 sorption and desorption of all the chemisorption‐based technologies. As demonstrated in monoethanolamine (MEA) based CO2 capture, even with the addition of only 2000 ppm IL catalyst, the rate of CO2 desorption—the key to reducing the overall CO2 capture energy consumption or breaking the bottleneck of the state‐of‐the‐art technologies and Paris Agreement implementation—can be increased by 791% at 85 °C, which makes use of low‐temperature waste heat and avoids secondary pollution during CO2 capture feasible. Furthermore, the catalytic CO2 capture mechanism is experimentally and theoretically revealed.