| Summary: | Composite solid electrolytes (CSEs), composed of sodium superionic conductor (NASICON)-type Li<sub>1+x</sub>Al<sub>x</sub>Ti<sub>2‒x</sub>(PO<sub>4</sub>)<sub>3</sub> (LATP), poly (vinylidene fluoride-hexafluoro propylene) (PVDF-HFP), and lithium bis (trifluoromethanesulfonyl)imide (LiTFSI) salt, are designed and fabricated for lithium-metal batteries. The effects of the key design parameters (i.e., LiTFSI/LATP ratio, CSE thickness, and carbon content) on the specific capacity, coulombic efficiency, and cyclic stability were systematically investigated. The optimal CSE configuration, superior specific capacity (~160 mAh g<sup>−1</sup>), low electrode polarization (~0.12 V), and remarkable cyclic stability (a capacity retention of 86.8%) were achieved during extended cycling (>200 cycles). In addition, with the optimal CSE structure, a high ionic conductivity (~2.83 × 10<sup>−4</sup> S cm<sup>−1</sup>) was demonstrated at an ambient temperature. The CSE configuration demonstrated in this work can be employed for designing highly durable CSEs with enhanced ionic conductivity and significantly reduced interfacial electrolyte/electrode resistance.
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