A Bifunctional Interface Enabling Stable Zinc Metal Batteries Across a Wide Depth‐of‐Discharge Window

ABSTRACT Zinc metal negative electrodes are attractive for batteries due to their commercial availability, high specific capacity, and low cost. However, uncontrollable dendrite growth and corrosion limit battery performance. This work introduces a bifunctional interface of Ag nanoparticles (NPs) embedded in a laser‐scribed reduced graphene oxide (rGO) framework on Zn metal (Ag‐rGO@Zn). The conductive rGO framework provides continuous electron‐transport pathways and reduces interfacial polarization, while the Ag NPs act as zincophilic nucleation sites that guide Zn deposition toward Ag‐containing regions. This interface promotes Zn ²⁺ transport, suppresses side reactions, and stabilizes Zn plating/stripping. Ag‐rGO@Zn exhibits a high Zn ²⁺ transference number of 0.75 and a reduced activation energy of 30.1 kJ mol ⁻¹ . In symmetric cells, Ag‐rGO@Zn maintains stable cycling for 2240 h at 3 mA cm ⁻² and 1 mAh cm ⁻² , and achieves 515 h at 28% depth of discharge, far exceeding bare Zn. X‐ray photoelectron spectroscopy (XPS) and time‐of‐flight secondary ion mass spectrometry (TOF‐SIMS) confirm the Ag‐guided Zn deposition behavior. Paired with a commercial MnO ₂ positive electrode, Ag‐rGO@Zn delivers improved capacity, reduced polarization, and enhanced cycling stability. Moreover, in a flexible pouch cell, the device demonstrates stable cycling under various bending angles, demonstrating the practical, scalable approach toward next‐generation flexible zinc‐ion energy storage.