Amphiphilic Interfacial Environment Reconfiguration Unlocks Long‐Life Zinc‐Ion Batteries With Lean Electrolytes and Ultra‐Low N / P Ratios

Water‐induced parasitic reactions and dendrite growth severely limit the performance of aqueous zinc‐ion batteries (AZIBs), particularly under practical conditions with ultra‐low negative/positive ( N / P ) ratios and electrolyte/capacity ( E / C ) ratios. Herein, a trace amount of amphiphilic carbinol (hydroxyl) terminated polydimethylsiloxane (CTP) is employed to reconfigure the interfacial charge environment at the Zn anode. The hydrophobic Si─O backbone of the CTP molecule adsorbs directionally onto the Zn surface through electrostatic forces, which facilitates compact coverage on the anode and effectively blocks the interfacial H 2 O contact to suppress parasitic reactions. Furthermore, theoretical calculations reveal that CTP exhibits high permanent and asymmetric dipole moments, serving as a highly efficient interfacial charge regulator. Upon capturing Zn 2+ by the hydrophilic hydroxyl groups, the CTP molecules effectively mediate interfacial charge distribution and electron transfer kinetics, thus promoting uniform Zn deposition. Consequently, the Zn//NH 4 V 4 O 10 battery exhibits exceptional cycling stability over 800 cycles at 0.5 A g −1 with a limited N / P ratio of 1.3 and E / C ratio of 15.84 µL mAh −1 . This work highlights the significance of constructing dipole‐mediated amphiphilic interfacial environments for advancing practical AZIBs under harsh working conditions.