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The practical application of AZIBs is hindered by problems such as dendrites and hydrogen evolution reactions caused by the thermodynamic instability of Zinc (Zn) metal. Modification of the Zn surface through interface engineering can effectively solve the above problems. Here, sulfonate‐derivatized graphene–boronene nanosheets (G&B‐S) composite interfacial layer is prepared to modulate the Zn plating/stripping and mitigates the side reactions with electrolyte through a simple and green electroplating method. Thanks to the electronegativity of the sulfonate groups, the G&B‐S interface promotes a dendrite‐free deposition behavior through a fast desolvation process and a uniform interfacial electric field mitigating the tip effect. Theoretical calculations and QCM‐D experiments confirmed the fast dynamic mechanism and excellent mechanical properties of the G&B‐S interfacial layer. By coupling the dynamics‐mechanics action, the G&B‐S@Zn symmetric battery is cycled for a long‐term of 1900 h at a high current density of 5 mA cm−2, with a low overpotential of ≈30 mV. Furthermore, when coupled with the LMO cathode, the LMO//G&B‐S@Zn cell also exhibits excellent performance, indicating the durability of the G&B‐S@Zn anode. Accordingly, this novel multifunctional interfacial layer offers a promising approach to significantly enhance the electrochemical performance of AZIBs. A simple and green electroplating method is employed to prepare the G&B‐S composite interfacial layer, regulating the Zn plating/stripping and mitigating the side reactions. Based on the dynamics‐mechanics coupling action, the G&B‐S@Zn symmetric battery can achieve long‐term cycling stability of 1900 h at 5 mA cm−2 with a small overpotential of ≈30 mV.