Full‐Chain Regulation Across Anode‐Electrolyte‐Cathode Enables High‐Capacity and Durable Aqueous Zn‐Te Batteries

ABSTRACT Aqueous zinc‐tellurium (Zn‐Te) batteries hold great potential in large‐scale energy storage owing to intrinsic safety and high theoretical capacity, yet their application is seriously hindered by sluggish Te redox kinetics and insufficient stability of Zn metal anodes. Herein, we use multifunctional choline iodide (ChI) to establish full‐chain regulation across the anode‐electrolyte‐cathode interface, thereby achieving a high‐performance Zn‐Te battery. It is revealed that preferentially absorbed Ch ⁺ ions form a water‐deficient Helmholtz inner layer at the anode, stabilizing the electrode‐electrolyte interface and promoting I ⁻ aggregation to enhance Zn ²⁺ migration kinetics. In the bulk electrolyte, Ch ⁺ suppresses water reactivity and cooperates with I ⁻ to optimize Zn ²⁺ solvation structure. Simultaneously at the cathode, I ⁻ catalyzes multi‐electron transfer reactions of Te and contributes additional capacity via redox activity, while Ch ⁺ coordinates with generated iodine species to stabilize Coulombic efficiency. Consequently, Zn symmetric cells exhibit stable cycling over 8400 h under 1 mA cm ⁻² /1 mAh cm ^−2, and Zn//Te@EG full cells deliver a high specific capacity of 423.8 mAh g ⁻¹ after 500 cycles at 1 A g ⁻¹ . Notably, at a practical N/P ratio of 2.78, the Zn//Te@EG full cell retains a high capacity of 581.3 mAh g ⁻¹ after 60 cycles at 0.2 A g ⁻¹ .