Reliable and Reusable All‐Solid‐State Contact‐Type Pre‐Lithiation Platform for High‐Performance All‐Solid‐State Batteries

All-solid-state batteries represent a promising approach for achieving high energy density and enhanced safety by utilizing bipolar cell architectures and nonflammable solid electrolytes. However, lithium loss during initial cycling occurs primarily due to the limited electrochemical stability of solid electrolytes and the irreversibility of anode materials with high theoretical capacities, resulting in a lower achievable energy density than theoretically expected. Additionally, all-solid-state batteries are highly sensitive to interfacial phenomena, which makes addressing these challenges crucial for maximizing their electrochemical performance. In this study, we introduce a reliable and reusable contact-type pre-lithiation platform specifically designed for all-solid-state systems. This platform, consisting of solid electrolytes and electron-conductive agents, exhibits balanced ionic and electronic transport characteristics, enabling uniform pre-lithiation of all-solid-state electrodes through simple, reversible physical contact. Even under a low stack pressure of 8 MPa, pre-lithiation can be effectively controlled by contact time and operating temperature, while the low stack pressure effectively suppresses the formation of highly resistive decomposition products at the interface. Consequently, the precisely pre-lithiated anodes with optimized interfacial characteristics significantly enhance Coulombic efficiency during initial cycles and overall cycling performance, contributing to the realization of high-performance all-solid-state batteries with genuinely high energy density.