Abstract: | The self‐healing of zinc‐ion batteries (ZIBs) will not only significantly improve the durability and extend the lifetime of devices, but also decrease electronic waste and economic cost. A poly(vinyl alcohol)/zinc trifluoromethanesulfonate (PVA/Zn(CF3SO3)2) hydrogel electrolyte was fabricated by a facile freeze/thaw strategy. PVA/Zn(CF3SO3)2 hydrogels possess excellent ionic conductivity and stable electrochemical performance. Such hydrogel electrolytes can autonomously self‐heal by hydrogen bonding without any external stimulus. All‐in‐one integrated ZIBs can be assembled by incorporating the cathode, separator, and anode into hydrogel matrix since the fabrication of PVA/Zn(CF3SO3)2 hydrogel is a process of converting the liquid to quasi‐solid state. The ZIBs show an outstanding self‐healing and can recover electrochemical performance completely even after several cutting/healing cycles. |