A Water‐Repellent‐Zincophilic Molecular Strategy for Concurrent Solvation and Interfacial Regulation toward Highly Reversible Zinc Anodes

ABSTRACT Aqueous zinc‐ion batteries are promising for grid‐scale energy storage but suffer from severe anode issues, including dendrite growth and water‐induced side reactions. Herein, an organic molecule, N,N,N’,N’‐Tetrakis(2‐hydroxyethyl)adipamide (THEA), is used to implement a “water‐repellent‐zincophilic” strategy for synergistically regulating both the electrolyte and the electrode interface. Its flexible hydrophobic backbone and multiple zincophilic hydroxyl groups enable multi‐site functionality. In the electrolyte, THEA coordinates with Zn 2+ to reconstruct the primary solvation sheath, displacing water, and reducing its activity. At the anode interface, it chemically adsorbs to form an organic interfacial layer. This layer effectively repels water to mitigate parasitic reactions while guiding Zn 2+ flux toward the dense (002) plane deposition. Consequently, cells employing THEA achieve exceptional stability: Zn||Zn cells cycle for over 5550 h (0.5 mA cm −2 , 0.5 mAh cm −2 ); Zn||β‐MnO 2 cells retain 81.3% capacity after 1000 cycles (1 A g −1 ) and 60.5% capacity after 3000 cycles at 2 A g −1 . Furthermore, THEA effectively suppresses ice crystallization at subzero temperatures, enabling stable Zn anode operation at −8°C. This work integrates solvation control with interfacial engineering, offering an effective pathway toward durable, high‐performance aqueous zinc batteries.