The PDF file includes:

• Fig. S1. Contact angle measurement of the polymer precursor and LE on the different substrates.
• Fig. S2. GC-MS of mixed gases.
• Fig. S3. Thermogravimetric analysis and differential scanning calorimetry curves of LiPF₆.
• Fig. S4. Effect of H₂O content on polymerization.
• Fig. S5. Polymerization mechanism of DOL induced by LiPF₆.
• Fig. S6. XPS spectra of LiPF₆ and GPE.
• Fig. S7. ¹³C NMR spectrum of PDXL (deuterated chloroform as solvent).
• Fig. S8. FTIR spectrum of PDXL.
• Fig. S9. Characteristic changes of GPE during the whole polymerization progress.
• Fig. S10. EIS curves of the GPE with various DME content in the precursors.
• Fig. S11. Volatilization property of GPE and LE.
• Fig. S12. Thermal analysis of the PDXL and polyethylene oxide (PEO).
• Fig. S13. Electrochemical tests of the Li-Cu batteries with GPE and LE.
• Fig. S14. Cross-sectional SEM image of the as-prepared cathode and separator soaked with GPE.
• Fig. S15. EIS and anode SEM images of Li-S batteries with GPE and LE.
• Fig. S16. XPS of the Li anodes of the Li-S batteries with GPE and LE after 50 cycles at 0.5 C.
• Fig. S17. Self-discharge tests and soft-package Li-S battery.
• Fig. S18. Charge/discharge curves of LiFePO₄|LE|Li battery.
• Fig. S19. Mechanical property of GPE with a special shape at room temperature.
• Table S1. Polymerization conversion rate of DOL in the electrolyte from monomer to polymer.
• Table S2. Ion conductivity of GPE with various DME content in the precursors.

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Other Supplementary Material for this manuscript includes the following:

• Movie S1 (.mp4 format). Contact angle measurement of polymer precursor and LE on cathode substrates.