The solid-state electrolytes (SSEs) are considered as a decent solution to rationally supersede the liquid one for the sake of dependable operation security and higher energy density when it comes to the next-generation lithium (Li) metal batteries. Herein, a sort of composite solid electrolyte with in-built ion-conductive 3D framework is designed to enable the stable performances of Li-metal batteries. The framework comprised of the Li⁺-conducting garnet components (Li_6.75La₃Zr_1.75Nb_0.25O₁₂, LLZN) and polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) provides the vulnerable part with mechanical support and well-behaved electrochemical stability. Stemmed from this embedded framework, the whole electrolyte exhibits high Li⁺ conductivity (4.6×10⁻⁴ S cm⁻¹), improved high-voltage endurance (4.4 V versus Li/Li⁺), better Li-anode compatibility and high-temperature feasibility. Additionally, the synergistic enhancements between LLZN and PVDF-HFP potentially facilitate the homogeneous ionic flux, thereby resulting in the persistence of a sound solid-electrolyte interphase. The solid-state batteries assembling composite solid electrolyte also deliver the preferable battery performance, featuring high-capacity output with stable cyclability. Application of this electrolyte in a pouch cell further demonstrates its feasibility and flexibility. This design concept is anticipated to give the way of exploring brand new solid electrolytes and boosting their overall electrochemical performances toward practicality.

对于下一代锂 (Li) 金属电池，固态电解质 (SSE) 被认为是合理取代液态电解质的理想解决方案，以实现可靠的运行安全性和更高的能量密度。在此，设计了一种具有内置离子导电 3D 框架的复合固体电解质，以实现锂金属电池的稳定性能。该框架由 Li ⁺导电石榴石成分 (Li _6.75 La ₃ Zr _1.75 Nb _0.25 O ₁₂ , LLZN) 和聚偏二氟乙烯-六氟丙烯 (PVDF-HFP) 为易损部分提供机械支撑和良好的电化学稳定性。源于这种嵌入框架，整个电解质表现出高 Li ⁺电导率（4.6×10 ^-4  S cm ^-1），提高了高压耐久性（4.4 V vs Li/Li ⁺），更好的锂负极相容性和高温可行性。此外，LLZN 和 PVDF-HFP 之间的协同增强可能促进均匀的离子通量，从而导致良好的固体电解质界面的持久性。组装复合固体电解质的固态电池也具有良好的电池性能，具有高容量输出和稳定的循环性能。这种电解质在软包电池中的应用进一步证明了其可行性和灵活性。预计这种设计理念将为探索全新的固体电解质并提高其整体电化学性能向实用性提供途径。