Carbon fibers have the combined mechanical and electrochemical properties needed to make them particularly well suited for usage as electrodes in a structural lithium-ion battery, a material that simultaneously works as a battery and a structural composite. Presented in this paper is an evaluation of commercial polyacrylonitrile-based carbon fibers in terms of capacity and coulombic efficiency, as well as a microstructural and surface evaluation. Some polyacrylonitrile based carbon fibers intercalate lithium ions, resulting in a similar capacity as state-of-the-art graphite based electrodes, presently the most commonly used negative electrode material. Using high precision coulometry, we found a capacity of around 250-350 mAh/g and a very high coulombic efficiency of over 99.9% after ten cycles, which is even higher than a commercial state-of-the art graphitic electrode evaluated as reference. The high coulombic efficiency is attributed to the very low surface area of the carbon fibers, resulting in a small and stable solid-electrolyte interface layer. A highly graphitized ultra high modulus carbon fiber was evaluated as well and, compared to the other fibers, less lithium was inserted (corresponding to approximately 150 mAh/g). We show that the use of carbon fibers as an electrode material in a structural composite battery is indeed viable. The demand for new and improved battery technologies is continuously rising. In particular the electrification of the transportation sector needs innovative new solutions to develop and meet new demands. Much research is dedicated to pushing the limits of lithium (Li)-ion batteries in terms of energy, power, safety, cost, lifetime and environmental aspects.Improving graphite and other carbon based electrodes has been extensively researched since the beginning of the 90s since they are the dominating type of negative electrodes in Li-ion batteries.1-5 Another way of improving the effectiveness at a system level is through so called multifunctional battery technologies. The idea is to let the battery perform several functions, in particular carry a mechanical load and still maintain the energy storage function. The weight at a system level can be reduced, and a performance enhancement can be achieved, even if the battery function is not on par with conventional state of the art Li-ion batteries. Batteries could be included as an integral part of the structure in different kinds of vehicles, such as cars or even airplanes. Multifunctionality of materials for battery and capacitor applications has been researched in various ways for a number of years. [6][7][8][9][10][11][12][13]