Owing to the promise of high safety and energy density, all‐solid‐state batteries are attracting incremental interest as one of the most promising next‐generation energy storage systems. However, their widespread applications are inhibited by many technical challenges, including low‐conductivity electrolytes, dendrite growth, and poor cycle/rate properties. Particularly, the interfacial dynamics between the solid electrolyte and the electrode is considered as a crucial factor in determining solid‐state battery performance. In recent years, intensive research efforts have been devoted to understanding the interfacial behavior and strategies to overcome these challenges for all‐solid‐state batteries. Here, the interfacial principle and engineering in a variety of solid‐state batteries, including solid‐state lithium/sodium batteries and emerging batteries (lithium–sulfur, lithium–air, etc.), are discussed. Specific attention is paid to interface physics (contact and wettability) and interface chemistry (passivation layer, ionic transport, dendrite growth), as well as the strategies to address the above concerns. The purpose here is to outline the current interface issues and challenges, allowing for target‐oriented research for solid‐state electrochemical energy storage. Current trends and future perspectives in interfacial engineering are also presented.

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We report a novel succinonitrile (SN)-based electrolyte SN–DLi–FEC (SN–LiTFSI–LiODFB–FEC), which shows excellent compatibility with the Li-metal anode.

Solid‐state electrolytes (SSEs) are attracting growing interest for next‐generation Li‐metal batteries with theoretically high energy density, but they currently suffer from safety concerns caused by dendrite growth, hindering their commercial applications. Interfaces between SSEs and solid lithium are argued to be crucial, affecting dendrite growth and determining solid‐state batteries (SSBs) performance. The buried and localized nature of the interface poses a huge challenge for direct characterization under working conditions. Recent review articles have been devoted to evaluating the conductivity and chemical stability of SSEs. Recognizing this, in this Review, the focus is on understanding lithium dendrite beyond conventional factors and offering a perspective on various surface/interface and microstructural phenomena that require close attention by both experimentalists and theoreticians. The complicated ion‐transport mechanism and chemomechanical information correlated with interface and lithium dendrite are discussed. Rational solutions are provided to engineer functional interfaces to suppress lithium dendrites and accelerate progress towards the commercialization of SSBs.

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Li7La3Zr2O12-based garnet (LLZO-BG) electrolyte has the advantage of strong thermal stability and hence can avoid the flammability problem of organic electrolyte solution. However, the solid-state lithium battery with LLZO-BG electrolyte...