Polytetrafluoroethylene (PTFE)-bonded gas-diffusion electrodes (GDEs), modified with polyaniline as an electron and proton conductor in the catalyst layer, are prepared and evaluated for use in proton-exchange membrane fuel cells (PEMFCs). Polyaniline is coated on the GDE by electropolymerization of aniline and trifluoromethane sulfonic acid as the proton-conductive monomer. The electrodes are characterized by cyclic voltammetry, current–potential measurements, electrochemical impedance spectroscopy, and chronoamperometry. The polyaniline is found to be homogenously dispersed in the catalyst layer, making it a good candidate proton and electron conductor. Use of polyaniline instead of Nafion in the catalyst layer, increases the utility of the electrocatalyst by 18%. The results are consistent with the presence of polyaniline as a conductive polymer in the reaction layer reducing the polarization resistance of the electrode in comparison with that of a corresponding electrode containing Nafion. Thus, the present results indicate that PEMFCs using polyaniline-containing electrocatalysts should give superior performance to those using catalysts containing traditional ionomers.