As emerging eutectic mixtures, deep eutectic electrolytes (DEEs) show unique properties for Li-metal batteries (LMBs). However, the limited choice and inferior electrode compatibility hinder their further development in LMBs. Herein, we report a new 1,2dimethylimidazole (DMIm)-based deep eutectic gel polymer electrolyte induced by LiÀ N interaction. We demonstrate that incorporating electron-withdrawing polyvinylidene difluoride (PVDF) polymer into the DMIm-based DEE changes the coordination environment of Li + ions, leading to a high transference number of Li + ions (0.65) and superior interface stability between the electrolyte and Li anode. The deep eutectic gel polymer electrolyte exhibits excellent non-flammability, high ionic conductivity (1.67 mS cm À 1 at 30 °C), and high oxidation voltage (up to 4.35 V vs. Li/Li + ). The Li j j LFP cell based on the newly developed deep eutectic gel polymer electrolyte can achieve superior long-term cycling stability at a wide range of rates.

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As emerging eutectic mixtures, deep eutectic electrolytes (DEEs) show unique properties for Li-metal batteries (LMBs). However, the limited choice and inferior electrode compatibility hinder their further development in LMBs. Herein, we report a new 1,2dimethylimidazole (DMIm)-based deep eutectic gel polymer electrolyte induced by LiÀ N interaction. We demonstrate that incorporating electron-withdrawing polyvinylidene difluoride (PVDF) polymer into the DMIm-based DEE changes the coordination environment of Li + ions, leading to a high transference number of Li + ions (0.65) and superior interface stability between the electrolyte and Li anode. The deep eutectic gel polymer electrolyte exhibits excellent non-flammability, high ionic conductivity (1.67 mS cm À 1 at 30 °C), and high oxidation voltage (up to 4.35 V vs. Li/Li + ). The Li j j LFP cell based on the newly developed deep eutectic gel polymer electrolyte can achieve superior long-term cycling stability at a wide range of rates.