Framework Integration for Adaptive Interfaces in Flexible Solid‐State Lithium–Oxygen Batteries

Abstract Lithium–oxygen batteries (LOBs), with their remarkable energy density, represent a pivotal advancement in energy storage technology. However, conventional Li–O 2 batteries face significant obstacles. This study introduces polyacrylonitrile (PAN)‐based polymer membranes and self‐supporting cathodes fabricated via electrospinning and thermal treatment. By incorporating poly(diallyldimethylammonium chloride) (PDDA)‐functionalized cathodes through electrostatic adsorption, a polymeric electrolyte‐functional integrated linkage structure was developed. This design facilitates adaptive interface modulation, creating a stable low‐impedance interface between the electrolyte and cathode while enabling efficient ion and electron transport. The resulting solid‐state LOBs (SSLOBs) demonstrate exceptional performance, achieving a specific capacity of 8600 mAh g −1 and a cycling lifespan of 191 cycles. The adaptive interface provides abundant reaction sites, promoting uniform ring‐like discharge product growth and reversible decomposition. Additionally, flexible batteries incorporating this structure exhibit outstanding resilience to bending deformation. These advancements highlight the transformative potential of Li–O 2 batteries, offering promising directions for future energy storage research.