Electropolymn. of 3,4-ethylenedioxythiophene (EDOT) was performed in an aq. micellar soln. onto conducting glass and conducting flexible plastic substrates using a simple, scalable process. The background electrolyte in the process consisted merely of a micellar aq. Na dodecyl sulfate (SDS) soln. Electrodeposition of poly(3,4-ethylenedioxythiophene) (PEDOT) was conducted at const. current, resulting in homogeneous films, even on large sized conducting glass and plastic substrates (9 cm × 9 cm). The use of H2O as electrolyte, application on large substrates and applicability on flexible plastic substrates demonstrates the feasibility of this method for upscaling and use in industrial fabrication of DSCs. DSCs were assembled using three different PEDOT thicknesses on conducting glass as counter electrodes and a comparison was made with thermally platinized conducting glass counter electrodes. In Co tris(bipyridine)-based electrolyte, the catalytic performance of the PEDOT counter electrodes was significantly higher than that of platinized counter electrodes. DSCs with PEDOT counter electrodes gave higher efficiencies due to higher fill factors and a lower charge transfer resistance. The low charge transfer resistance and good catalytic performance of the PEDOT counter electrodes can be related to its mesoporous morphol. resembling crumpled sheets of paper.