Carbonic anhydrase (CA) is a zinc-containing metalloprotein, in which the Zn active center plays the key role to transform CO2 into carbonate. Inspired by nature, herein we used metal-organic frameworks (MOFs) to mimic CA for CO2 conversion, on the basis of the structural similarity between the Zn coordination in MOFs and CA active center. The biomimetic activity of MOFs was investigated by detecting the hydrolysis of para-nitrophenyl acetate, which is a model reaction used to evaluate CA activity. The biomimetic materials (e.g., CFA-1) showed good catalytic activity, and excellent reusability, and solvent and thermal stability, which is very important for practical applications. In addition, ZIF-100 and CFA-1 were used to mimic CA to convert CO2 gas, and exhibited good efficiency on CO2 conversion compared with those of other porous materials (e.g., MCM-41, active carbon). This biomimetic study revealed a novel CO2 treatment method. Instead of simply using MOFs to absorb CO2, ZIF-100 and CFA-1 were used to mimic CA for in situ CO2 conversion, which provides a new prospect in the biological and industrial applications of MOFs.