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Using a three-dimensional (3D) Li-ion conducting ceramic network, such as Li7La3Zr2O12 (LLZO) garnet-type oxide conductor, has proved to be a promising strategy to form continuous Li ion transfer paths in a polymer-based composite. However, the 3D network produced by brittle ceramic conductor nanofibers fails to provide sufficient mechanical adaptability. In this manuscript, we reported a new 3D ion-conducting network, which is synthesized from highly loaded LLZO nanoparticles reinforced conducting polymer nanofibers, by creating a lightweight continuous and interconnected LLZO-enhanced 3D network to outperform conducting heavy and brittle ceramic nanofibers to offer a new design principle of composite electrolyte membrane featuring all-round properties in mechanical robustness, structural flexibility, high ionic conductivity, lightweight, and high surface area. This composite-nanofiber design overcomes the issues of using ceramic-only nanoparticles, nanowires, or nanofibers in polymer composite electrolyte, and our work can be considered as a new generation of composite electrolyte membrane in composite electrolyte development.

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