Zhe Li, Kai Chen, Tianyun Jing, Naijia Zhao, Xinyan Jiang, Jia Ge, Junzhu Tao, Yu Zhang, Jiacheng Hu, Shuqi Wang, Yue Wang, Liwen Xie, Yifan Guo, Xi Wang, Ziqi Ren, Jian Zhang, Lei Jiang, Zhen Zhang
ABSTRACT Enhancing the performance of ion‐selective membranes is critical for achieving efficient osmotic energy conversion. However, existing charge‐regulation strategies struggle to adapt to dynamically changing ion‐transport environments. Inspired by natural cytochrome c oxidase (C c O), this work demonstrates that atomically precise heteronuclear FeCo dual‐atom nanozymes (FeCo‐DACs) can dynamically modulate the local charge distribution at active sites via an oxidase‐like mechanism, thereby enhancing osmotic energy conversion. By tailoring the coordination environments of heteronuclear and homonuclear dual‐atom sites, enzyme‐like activity and ion selectivity are optimized. The bioinspired composite membrane incorporating Fe─Co bonded nanozymes directly into bacterial cellulose (BC/FeCo‐DACs) achieves a power density of 15.4 W m −2 during the mixing of natural river water and seawater, without external stimuli. Combined experimental and theoretical analyses reveal that the heteronuclear FeCo configuration, with an optimal metal–metal bond length, balances oxygen adsorption/desorption while establishing the most energetically favorable proton‐consumption pathway, enabling spontaneous dynamic local charge regulation and improved osmotic energy conversion performance.