Bio‐Inspired Nucleotide Electrolyte Engineering Enables Highly Reversible Zinc Anodes for Aqueous Zinc‐Ion Batteries

ABSTRACT Aqueous zinc‐ion batteries (AZIBs) are promising for large‐scale energy storage but suffer from Zn dendrite growth, water‐induced parasitic reactions, and interfacial instability. Herein, inspired by natural nucleotide architectures, we introduce disodium inosinate (IMP) as a green multifunctional electrolyte additive to regulate Zn electrochemistry. Its naturally preorganized nucleotide framework integrates chemically differentiated phosphate, hydroxyl‐rich ribose, and O/N‐containing heterocyclic regions, which exhibit distinct interaction preferences toward Zn 2 + , water molecules, and the Zn surface under different local electrochemical environments. Experimental and theoretical studies reveal that IMP participates in Zn 2+ solvation and regulates the local water environment, while preferential multisite adsorption at the Zn interface homogenizes Zn 2+ flux and promotes Zn(002)‐preferred deposition, enabling dense and dendrite‐suppressed Zn growth. Consequently, Zn||Zn cells achieve stable cycling for over 2000 h at 5 mA cm −2 and 2.5 mAh cm −2 , while Zn||Cu cells maintain an average Coulombic efficiency above 99.8% over 3500 cycles. Zn||NVO full cells retain 87.3% capacity after 2000 cycles at 4 A g −1 , and pouch cells demonstrate stable cycling for 300 cycles. This work highlights how the intrinsic chemical differentiation of a naturally preorganized nucleotide architecture can translate into distinct molecular interactions across different electrochemical environments, providing a bio‐inspired strategy for sustainable aqueous electrolyte design.