Harmonizing Enzyme‐like Cofactors to Boost Nanozyme Catalysis

Abstract Engineering isolated metal sites resembling the primary coordination sphere of metallocofactors enables atomically dispersed materials as promising nanozymes. However, most existing nanozymes primarily focus on replicating specific metallocofactors while neglecting other supporting cofactors within active pockets, leading to reduced electron transfer (ET) efficiency and thus inferior catalytic performances. Herein, we report a metal–organic framework UiO‐67 nanozyme with atomically dispersed iron sites, which involves multiple tailored enzyme‐like nanocofactors that synergistically drive the ET process for enhanced peroxidase‐like catalysis. Among them, the linker‐coupled atomic iron site plays a critical role in substrate activation, while bare linkers and zirconia nodes facilitate the ET efficiency of intermediates. The synergy of three nanocofactors results in a 4.29‐fold enhancement compared with the single effort of isolated metal site‐based nanocofactor, holding promise in immunoassay for sensitive detection of chlorpyrifos. This finding opens a new way for designing high‐performance nanozymes by harmonizing various nanocofactors at the atomic and molecular scale.