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Polyethylenimine (PEI)‐grafted silica nanoparticles were fabricated and characterized for the electrostatic immobilization of a CO2 conversion enzyme. PEI was supposed to serve as a carbonic anhydrase mimic for CO2 capture and conversion to HCO3− (the optimal substrate of many CO2 conversion enzymes) and was proved to assist phosphoenolpyruvate carboxylase to form a dual‐enzyme cascade system for...