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Structural batteries, also known as “massless batteries”, integrate energy storage directly into load-bearing materials, offering a transformative alternative to traditional Li-ion batteries. Unlike conventional systems that serve only as energy storage devices, structural batteries replace passive structural components, reducing overall weight while providing mechanical reinforcement. However, achieving uniform and efficient coatings of active materials on carbon fibers remains a major challenge, limiting their scalability and electrochemical performance. This study investigates ultrasonic spray coating as a precise and scalable technique for fabricating composite cathodes in structural batteries. Using a computer-controlled ultrasonic nozzle, this method ensures uniform deposition with minimal material waste while maintaining the mechanical integrity of carbon fibers. Compared to traditional techniques such as electrophoretic deposition, vacuum bag hot plate processing, and dip-coating, ultrasonic spray coating achieved superior coating consistency and reproducibility. Electrochemical testing revealed a specific capacity of 100 mAh/gLFP with 80% retention for more than 350 cycles at 0.5 C, demonstrating its potential as a viable coating solution. While structural batteries are not yet commercially viable, these findings represent a step toward their practical implementation. Further research and optimization will be essential in advancing this technology for next-generation aerospace and transportation applications.