In this work, an "upright" cellulose layered template, which can be precisely controlled by the fiber orientation and thickness of anisotropic cellulose film, was first developed to prepare vertically aligned Li 7 La 3 Zr 2 O 12 (LLZO) ceramic membrane with low tortuosity and uniform porosity. The flexible composite solid-state electrolytes (CSEs) were synthesized by incorporating poly(ethylene oxide) (PEO) polymer into LLZO architecture, and exhibited distinguished mechanical strength, elevated ionic conductivity (2.1 Â 10 À4 S cm À1 ) and excellent interface compatibility with lithium anodes. The assembled LiFePO 4 / lithium full cells assembled with as-obtained CSEs can reach large discharge capacities of 172.3 mAh g À1 with coulombic efficiencies of above 99% and capacity retention of 93.1% even after 200 cycles. These results clearly demonstrate that the sophisticated design of vertical aligned cellulose layered template with fine-scale size and exquisite architecture is a promising and practical approach in fabricating flexible LLZO@PEO-LiTFSI CSEs with highsafety and high-performance.Hao Zhang and Xingye An contribute equally to this work as co-first authors. Thanks for the contributions of all of the co-authors and their friends.
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