Zinc metal is a high‐capacity and cost‐effective anode material for aqueous zinc‐ion batteries, but its development is impeded by dendrite growth and interfacial side reactions. In this study, a unique dipole molecule (DPM) layer is constructed on a zinc surface via an in situ etching‐growth strategy to regulate the surface electric field and ion distribution. Theoretical calculations and experiments confirm that the asymmetrical charge distribution within the DPM layer can significantly remodel the electric field of the Zn anode surface. The zincophilic DPM layer accelerates the migration of zinc ions through ordered ion channels. Electro‐ionic field regulation via the DPM layer achieves dendrite‐free deposition and reduces the formation of byproducts. The DPM‐Zn symmetrical cells exhibit ultralow voltage hysteresis (≈ 24.2 mV), highly reversible zinc plating/stripping behavior, and stable cycling over 1700 h at 1 mA cm−2. The DPM‐Zn||MnO2 full cells exhibited a higher specific capacity and cycle stability than the bare Zn anode. This work verifies the feasibility of electro‐ionic‐field synergistic regulation for robust Zn anodes and provides new insights into the interface design of metal anodes.