ABSTRACTAniline has been polymerized via electrodeposition onto various nonwoven carbon fiber fabric (CFF) substrates for use as a pseudocapacitive electrochemical capacitor. Four types of CFF were initially tested for double layer capacitance before polyaniline deposition, and again for specific capacitance after deposition. A binder‐free CFF was selected for further analysis due to its high capacitance change following PANI deposition (three orders of magnitude). The aniline monomer concentration, deposition potential, and deposition time were varied and resulting materials were characterized using chrono‐potentiometry, cyclic voltammetry, and scanning electron microscopy. The deposition potential range yielding highest capacitance was found to be between 0.744 and 0.777 V. A solution concentration of 0.5M aniline at a 20 min deposition time resulted in the highest specific capacitance (>80 F/g based on total electrode mass and >300 F/g based on PANI mass) within this study. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 43315.