The use of poly( 3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) in electrodes and electrical circuits presents a number of challenges that are yet to be overcome, foremost amongst which are its relatively low conductivity, low coatability on hydrophobic substrates, and decreased conductivity at large strains. With this in mind, this study suggests a simple way to simultaneously address all of these issues through the addition of a small amount of a nonionic surfactant (Triton X-100) to commercial PEDOT:PSS solutions. This surfactant is shown to considerably reduce the surface tension of the PEDOT:PSS solution, thus permitting conformal coatings of PEDOT:PSS thin film on a diverse range of hydrophobic substrates. Furthermore, this surfactant induces the formation of PEDOT nanofibrils during coating, which led to the high conductivity values and mechanical stability at large strains (epsilon = 10.3%). Taking advantage of the superior characteristics of these PEDOT:PSS thin films, a highly flexible polymer solar cell was fabricated. The power conversion efficiency of this solar cell (3.14% at zero strain) was preserved at large strains (epsilon = 7.0%).