Dynamic Interface Modulation of Aqueous Zinc–Ion Batteries by Rational Design of Organic Additives

Abstract Aqueous zinc–ion batteries (AZIBs) represent viable options for large‐scale energy storage, attributed to their high theoretical capacity, availability of resources, and intrinsic safety features. However, the zinc–water interface poses significant challenges including dendrite growth, hydrogen evolution, and corrosion, which considerably restrict battery performance. This review systematically examines organic additive strategies for zinc anode interface regulation in AZIBs. Structure–property relationships are established correlating molecular design with interfacial behavior through three fundamental mechanisms, which are electric double layer (EDL) modulation, solvation structure optimization via coordination effects, and controlled solid electrolyte interphase (SEI) formation. The review analyzes adsorption mechanisms of organic additives, distinguishing between physical adsorption‐based and SEI‐forming additives, where the former dynamically modulates the interfacial environment, while the latter establishes durable protective layers. Multifunctional additives integrating multiple regulatory mechanisms demonstrate superior performance optimization. Comparative analysis reveals that liquid organic additives excel in solvation structure regulation, whereas solid additives show advantages in interfacial adsorption and SEI engineering. Through systematic analysis of reported molecules, design principles are established linking molecular features to interfacial properties, providing guidance for rational development of next‐generation organic additives in high‐performance AZIBs.