Abstract:A novel multifunctional material has been designed to provide excellent mechanical properties whilst possessing a high electrochemical surface area suitable for electrochemical energy storage: structural carbon fibre fabrics are embedded in a continuous network of carbon aerogel (CAG) to form a coherent but porous monolith. The CAG-modification process was found to be scalable and to be compatible with a range of carbon fibre fabrics with different surface properties. The incorporation of CAG significantly increased the surface area of carbon fibre fabrics, and hence the electrochemical performance, by around 100-fold, resulting in a CAG-normalised specific electrode capacitance of around 62 Fg -1 , determined by cyclic voltammetry in an aqueous electrolyte. Using an ionic liquid (IL) electrolyte, the estimated energy density increased from 0.003 to 1 Whkg -1 , after introducing the CAG into the carbon fibre fabric. 'Proof-of-concept' multifunctional structural supercapacitor devices were fabricated using an IL-modified solid-state polymer electrolyte as a multifunctional matrix to provide both ionic transport and physical support for the primary fibres. Two CAG-impregnated carbon fabrics were sandwiched around an insulating separator to form a functioning structural electrochemical double layer capacitor composite.The CAG-modification not only improved the electrochemical surface area, but also reinforced the polymer matrix surrounding the primary fibres, leading to dramatic improvements in the matrix-dominated composite properties. Increases in in-plane shear strength and modulus, of up to 4.5-fold, were observed, demonstrating that CAG-modified structural carbon fibre fabrics have promise in both pure structural and multifunctional energy storage applications.3