Multifunctional structural batteries promise advancements in structural energy storage technologies by seamlessly integrating load-bearing and energy-storage functions within a single material, reducing weight, and enhancing safety. Yet, commercialization faces challenges in materials processing, assembly, and design optimization. Here, we report a systematic approach to develop a carbon fiber (CF)-based structural battery impregnated with epoxy-based solid polymer electrolyte (SPE) via robust vacuum-assisted compression molding (VACM). Informed by cure kinetics, SPE processing enhances the multifunctional performance with no fillers or additives. The thin flexible CF-based laminae impregnated under high pressure achieved a substantial enhancement of ∼160% in the fiber volume fraction (FVF) as although thin and strip-shaped, the fibers were optimally packed with low void. A CF/SPE-based battery was fabricated, with a hybrid layered ionic liquid (IL)/ carbonate electrolyte (CE) showing enhanced safety and multifunctional performance. Enhanced by thin, uniform, and stiff CF-based composites, this study propels the development of advanced multifunctional structures, thereby expediting sustainable commercialization.
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