Stable Zinc Deposition Enabled by Descriptor‐Guided Screening of Organic Electrolyte Additives Based on Molecular Polarizability and Surface Energy

Abstract Organic electrolyte additives have emerged as a promising strategy to regulate interfacial reactions at the Zn anode in aqueous batteries, yet their design remains largely empirical owing to a lack of molecular‐level understanding. In this work, a dual‐descriptor framework based on molecular polarizability and surface energy to guide the rational screening of electrolyte additives for stable Zn deposition is introduced. Systematic evaluation reveals that lower polarizability promotes the formation of a compact, water‐deficient electrical double layer (EDL), which enhances Zn 2+ desolvation and promotes rapid nucleation with oriented growth. Meanwhile, a moderately high surface energy, particularly when closely matched with that of the ZnSO 4 electrolyte, ensures stable interfacial adsorption and synergizes with low polarizability to achieve uniform Zn deposition. In contrast, excessively high surface energy induces additive aggregation, weakens EDL compactness, and leads to uneven deposition and parasitic side reactions. Guided by this dual‐descriptor screening framework, oxamide is identified as a representative additive featuring low polarizability and well‐matched surface energy. Its incorporation improves Zn deposition morphology, enhances coulombic efficiency, and delivers superior cycling stability in both half‐cell and Zn‐MnO 2 full‐cell configurations. This study demonstrates the effectiveness of descriptor‐guided additive design and offers a molecular‐level strategy for advancing stable and high‐performance aqueous Zn‐ion batteries.