The integration of Li S within a poly(ethylene oxide) (PEO)-based polymer electrolyte is demonstrated to improve the polymer electrolyte's ionic conductivity because the strong interplay between O and Li from Li S reduces the crystalline volume within the PEO. The Li/electrolyte interface is stabilized by the in situ formation of an ultra-thin Li S/Li S layer via the reaction between Li S and lithium metal, which increases the ionic transport at the interface and suppresses lithium dendrite growth. A symmetric Li/Li cell with the Li S -integrated composite electrolyte has excellent cyclability and a high critical current density of 0.9 mA cm at 40 °C. Impressive electrochemical performance is demonstrated with all-solid-state Li/LiFePO and high-voltage Li/LiNi Mn Co O cells at 40 °C.
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