Zn metals have gained the immense attention of researchers for their wide employment as the anode of high-performance aqueous batteries. Nonetheless, the Zn anodes suffer from uncontrollable dendrite growth and parasitic side reactions, which substantially shorten the battery lifespan. This study proposes an interfacial assembly of a metal-polyphenol coordination coating on Zn anodes to regulate Zn2+ deposition behavior. Bismush-coordinated polyphenolic ligands (i.e., tannic acid, TA) create a functional interface that could promote Zn's uniform nucleation and plating/striping kinetics. Moreover, the artificial coating acts as a physical barrier to inhibit surface corrosion. As a consequence, the TA-Bi-modified Zn anodes display a small voltage hysteresis of ~38 mV at 1 mA cm−2 over 2600 h and an ultra-long lifespan for 3100 h (~4.3 months) even at a high-current density of 10 mA cm−2. When assembled with a vanadium-based cathode, the full Zn-ion batteries achieve improved electrochemical performance.
