All-solid-state lithium batteries (ASSLBs) have the potential to revolutionize battery systems for electric vehicles due to their benefits in safety, energy density, packaging, and operable temperature range. As the key component in ASSLBs, inorganic lithium-ion-based solid-state electrolytes (SSEs) have attracted great interest, and advances in SSEs are vital to deliver the promise of ASSLBs. Herein, a survey of emerging SSEs is presented, and ion-transport mechanisms are briefly discussed. Techniques for increasing the ionic conductivity of SSEs, including substitution and mechanical strain treatment, are highlighted. Recent advances in various classes of SSEs enabled by different preparation methods are described. Then, the issues of chemical stabilities, electrochemical compatibility, and the interfaces between electrodes and SSEs are focused on. A variety of research addressing these issues is outlined accordingly. Given their importance for next-generation battery systems and transportation style, a perspective on the current challenges and opportunities is provided, and suggestions for future research directions for SSEs and ASSLBs are suggested.

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The logo of 110th Anniversary of Tongji University is represented using the crystal structure of garnet inorganic solid‐state electrolyte as units. In article number https://doi.org/10.1002/adma.201705702, Wei Luo, Yunhui Huang, and co‐workers summarize the recent progress on lithium‐based inorganic solid‐state electrolytes. The challenges and the corresponding advanced strategies for developing all‐solid‐state lithium batteries are highlighted. Image credit: Jiaqi Dai, University of Maryland.

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