Solid-state electrolytes have been widely investigated for lithium batteries since they provide a high degree of safety. However, their low ionic conductivity and substantial growth of lithium dendrites hamper their commercial applications. Garnet-type LiLaZrTaO (LLZTO) is one of the most promising active fillers to advance the performance of the solid polymer electrolyte. Nevertheless, their performance is still limited due to their large interfacial resistance. Herein, we embedded the amorphous LiO (LO) into LLZTO particles via the quenching process and successfully achieved an interfacial layer of LiO around LLZTO particles (LLZTO@LO). Amorphous LiO acts as a binder and showed an excellent affinity for Li ions which promotes their fast transference. Moreover, the stable and dense interfacial LiO layer enhances interfacial contact and suppresses the lithium dendrite growth during the long operation cycling process. The PEO/10LLZTO@2LO solid composite polymer electrolyte (SCPE) showed the highest ionic conductivity of 3.2 × 10 S cm at 40 °C as compared to pristine LLZTO-based SCPE. Moreover, the Li│(PEO/10LLZTO@2LO) │Li symmetric cell showed a stable and smooth long lifespan up to 1100 h at 40 °C. Furthermore, the LiFePO//Li full battery with PEO/10LLZTO@2LO SCPE demonstrated stable cycling performance for 400 cycles. These results constitute a significant step toward the practical application of solid-state lithium metal batteries (SS-LMBs).
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