| Summary: | Solid-state lithium metal batteries (LMBs) have been extensively investigated owing to their safer and higher energy density. In this work, we prepared a novel elastic solid-state polymer electrolyte based on an in situ-formed elastomer polymer matrix with ion-conductive plasticizer crystal embedded with Li<sub>6.5</sub>La<sub>3</sub>Zr<sub>1.5</sub>Ta<sub>0.5</sub>O<sub>12</sub> (LLZTO) nanoparticles, denoted as LZT/SN-SPE. The unique structure of LZT/SN-SPE shows excellent elasticity and flexibility, good electrochemical oxidation tolerance, high ionic conductivity, and high Li<sup>+</sup> transference number. The role of LLZTO filler in suppressing the side reactions between succinonitrile (SN) and the lithium metal anode and propelling the Li<sup>+</sup> diffusion kinetics can be affirmed. The Li symmetric cells with LZT/SN-SPE cycled stably over 1100 h under a current density of 5 mA cm<sup>−2</sup>, and Li||LiFePO<sub>4</sub> cells realized an excellent rate (92.40 mAh g<sup>−1</sup> at 5 C) and long-term cycling performance (98.6% retention after 420 cycles at 1 C). Hence, it can provide a promising strategy for achieving high energy density solid-state LMBs.
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