Geometry‐Regulated Electrode‐Wide Nucleation Patterns in Aqueous Zinc Anodes

ABSTRACT Zinc metal is a promising anode for aqueous zinc batteries due to its high theoretical capacity and low cost. However, its practical implementation remains limited by dendrite formation and interfacial instability. Herein, we present a geometry‐driven strategy that regulates Zn deposition through control of the hole opening ratio (HOR) in laser‐ablated three‐dimensional hole‐patterned Zn foil. Based on preferential Zn deposition at periodically arranged hole edges, HOR was introduced as a geometric parameter that dictates the spatial density of nucleation sites. Systematic variation of the HOR reveals that it governs the dispersion and size of early‐stage Zn deposits, defining the electrode‐wide nucleation pattern and subsequent growth behavior. The optimized HOR balances sparse nucleation with localized growth and dense nucleation with coalescence‐driven aggregation, enabling spatially uniform Zn deposition. As a result, the HOR‐tailored electrode achieves dendrite‐free deposition with long‐term stability in symmetric cells (3400 h at 0.5 mA cm −2 ) and maintains stable cycling in full cells paired with a Zn pre‐intercalated NH 4 V 4 O 10 cathode (1000 cycles at 2 A g −1 ). By establishing HOR‐controlled nucleation density as a geometry‐based design principle, this defect‐engineered and materials‐independent approach provides a general design framework for high‐performance aqueous metal batteries.