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All‐solid‐state thin‐film lithium batteries (TFLBs) are the ideal wireless power sources for on‐chip micro/nanodevices due to the significant advantages of safety, portability, and integration. As the bottleneck for increasing the energy density of TFLBs, the key components of cathode, electrolyte, and anode are still underway to be improved. In this review, a brief history of TFLBs is first outlined by presenting several TFLB configurations. Based on the state‐of‐the‐art materials developed for lithium‐ion batteries (LIBs), the challenges and related strategies for the application of those potential electrode and electrolyte materials in TFLBs are discussed. Given the advanced manufacture and characterization techniques, the recent advances of TFLBs are reviewed for pursuing the high‐energy‐density and long‐term‐durability demands, which could guide the development of future TFLBs and analogous all‐solid‐state lithium batteries. [ABSTRACT FROM AUTHOR]

Solid‐state lithium batteries (SSLBs) are promising owing to enhanced safety and high energy density but plagued by the relatively low ionic conductivity of solid‐state electrolytes and large electrolyte–electrode interfacial resistance. Herein, we design a poly(vinylidene fluoride‐co‐hexafluoropropylene) (PVDF‐HFP)‐based polymer‐in‐salt solid electrolyte (PISSE) with high room‐temperature ionic conductivity (1.24×10−4 S cm−1) and construct a model integrated TiO2/Li SSLB with 3D fully infiltration of solid electrolyte. With forming aggregated ion clusters, unique ionic channels are generated in the PISSE, providing much faster Li+ transport than common polymer electrolytes. The integrated device achieves maximized interfacial contact and electrochemical and mechanical stability, with performance close to liquid electrolyte. A pouch cell made of 2 SSLB units in series shows high voltage plateau (3.7 V) and volumetric energy density comparable to many commercial thin‐film batteries. [ABSTRACT FROM AUTHOR]