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Nanozymes hold great potential in nanomedicine, yet biotoxicity limits their clinical translation because of their uncontrolled catalytic activity, artificial inorganic components, and harsh synthesis conditions. Herein, a peroxidase‐like bionanozyme with ultrahigh and photocontrolled catalytic activity through the self‐assembly of biomolecules, hemin, and in situ polymerization of pyrrole in an aqueous...