The low ionic conductivity, poor interface contact, and low safety of the electrolytes are the main problems in the practical application in flexible lithium metal batteries. A new type of chemical crosslinked ionic gel polymer electrolyte (IGPE) with good self‐healing ability and excellent electrochemical properties is designed based on polyoxyethylenebis(amine), and 1,3,5‐benzenetricarboxaldehyde in the presence of ionic liquid through a one‐step reaction. The interaction between ionic liquid and polymer with the ether oxygen atom of EO chains improves the stability of IGPE and the crystallinity decreased significantly due to the incorporation of ionic liquid. The IGPEs show good self‐healing, film flexibility, and high ionic conductivity even at −25 °C. They also possess high thermal stability, wide electrochemical stability window, and good interfacial compatibility. The Li/IGPE‐50/LiFeO4 battery with IGPE‐50 as an electrolyte is studied and the high discharge capacity of 154.8 mAh g−1 is obtained at 0.1 C with 99.6% of coulombic efficiency, and remains 132.8 mAh g−1 on the 50th cycle. Ionic liquid combined with polymers based on dynamic reversible bonds can optimize the electrochemical performance of IGPEs, and improve its safety and stability, which is very useful for flexible lithium metal batteries.

All-solid polymer electrolytes with good self-healing ability and high stability were designed based on polyoxyethylenebis(amine) (H 2 N-PEG-NH 2 ) and 1,3,5-benzenetricarboxaldehyde through the Schiff base reaction. The effects of H 2 N-PEG-NH 2 of various molecule weights on thermal and electrochemical properties were studied. It was found that shCLSPE-3400 electrolyte with appropriate PEG chain simultaneously exhibited good thermal stability, excellent self-healing ability and high mechanical strength, which is due to the introduction of crosslinked network structure and dynamic reversible bonds in the electrolyte. It also showed a high ionic conductivity of 4.8 × 10 −4 S cm −1 , wide electrochemical stability window (5.1 V) and good lithium ion transfer number (t Li+ = 0.31) with an ethylene oxide/Li + ratio of 20:1 at 25 °C. In addition, a Li|shCLSPE-3400|LiFePO 4 battery with shCLSPE-3400 as electrolyte was studied, and it showed good reversible specific capacity. Such electrolyte has potential for application in solid-state batteries, which will facilitate improvement in the safety performance of lithium metal batteries.

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