Electrospinning was used to create custom-made fibrous electrode materials for redox flow batteries with targeted structural properties. The aim was to increase the available surface area for electrochemical reaction without diminishing the transport properties of the electrode. Electrospinning conditions were identified that could produce fibers several times larger than those typically yielded by the technique, yet much smaller than in commercially available electrodes. These materials were subsequently carbonized using widely reported protocols. The resultant materials were subjected to a range of characterization tests to confirm that the feasibility of the target material, including surface area, pore and fiber sizes, porosity, conductivity, and permeability. The most promising material to emerge from this selection processes was then tested for electrochemical performance in a flow cell. The produced material performed markedly better than a commercially available material. Further optimizations such as improved consistency in the production and some surface activation treatments could provide significant advancements. (C) The Author(s) 2017. Published by ECS. All rights reserved.