The method employed for depositing nanostructures of conducting polymers dictates potential uses in a variety of applications such as organic solar cells, light-emitting diodes, electrochromics, and sensors. A simple and scalable film fabrication technique that allows reproducible control of thickness, and morphological homogeneity at the nanoscale, is an attractive option for industrial applications. Here we demonstrate that under the proper conditions of volume, doping, and polymer concentration, films consisting of monolayers of conducting polymer nanofibers such as polyaniline, polythiophene, and poly(3-hexylthiophene) can be produced in a matter of seconds. A thermodynamically driven solution-based process leads to the growth of transparent thin films of interfacially adsorbed nanofibers. High quality transparent thin films are deposited at ambient conditions on virtually any substrate. This inexpensive process uses solutions that are recyclable and affords a new technique in the field of conducting polymers for coating large substrate areas.Marangoni | surface tension | thin film technology | organic electronics C onducting polymers hold promise as flexible, inexpensive materials for use in electronic applications including solar cells, light-emitting diodes, and chemiresistor-type sensors (1-3). Whereas traditional nonconjugated polymers are often solutionprocessable, many organic conducting polymers have been notoriously difficult to process into films. Thin films of conducting polymers offer a large ratio of charge carriers to volume of active layer (4) and can achieve high field-effect mobilities as a result of low-dimensional transport (5). Therefore a simple, scalable, cost-effective deposition technique for conducting polymers that produces a uniform thin film morphology reproducibly is needed.Film-forming methods for conducting polymers on the basis of solution processing, electrochemistry, and thermal annealing have been reported in the literature but suffer from a variety of problems. The conducting polymers polyaniline (PANi), polythiophene, and their derivatives such as poly(3-hexylthiophene) (P3HT) are commonly processed into nanoscale thin films via spin coating (1, 5-7) for applications in organic photovoltaics, thin film transistors, and electrochromic devices (8-12). However, spin coating is a technique that suffers from a low material utilization yield and is therefore not cost-effective (11), a fact that hinders its potential for scale-up. Another well known deposition strategy is the electrochemical growth of conducting polymer thin films via galvanostatic, potentiostatic, or voltammetric routes (9,(13)(14)(15)). An inherent limitation of using electricity for thin film deposition is the dual role played by the electrode/substrate, which excludes the possibility of film deposition on a nonconducting substrate. This problem also applies to electrospraying because it requires a high voltage across electrodes (11). Other solution-based methods also present challenges; for example, the Lang...