Abstract Carbonic anhydrase (CA) has demonstrated great potential to mitigate CO2 emissions by enzymatic conversion of CO2, while its commercial implementation is limited by the inherent shortcomings of CA, such as thermal and chemical instability, high sensitivity to the environment, and high cost. To overcome the drawbacks of CA and develop advanced technologies for mitigating CO2 emission, for the first time, mimetic CA (ZnHisGly) with the characteristics of natural CA was designed and synthesized, i.e., zinc-based deep eutectic solvent (DES), to boost CO2 hydration and conversion. The mimetic CA exhibited facile synthesis, high stability, and low cost as the characteristics of DES, and showed better catalytic performance compared to the currently reported mimetic CA. Particularly, its catalytic performance increased greatly with increasing pH and temperatures, which provides promising prospects in the industrial applications of DES-based CA mimics.