The discovery of organic electroluminescence (EL) in manufacturable small molecule [1] and p-conjugated polymer [2] thin-film format has led to the commercialization of organic light-emitting diode (OLED) technology and the development of many other novel semiconductor devices. One of the key goals for research in this field is high-performance, fully plastic electronic devices, but before such technology can be realized, organic electrode materials with conductivities and stabilities comparable to standard inorganic materials must be developed. Indium tin oxide (ITO) is the present industry standard transparent inorganic anode material for rigid devices, such as optical displays and solar cells. Attempts have also been made at implementing ITO in an emerging generation of flexible devices, but it is not an ideal choice owing to its inherent brittleness and susceptibility to conductivity changes after bending. [3][4][5] When this is considered alongside the ever-increasing cost of indium, it is clear that there is a pressing need to develop organic-based electrode materials for both flexible and rigid substrate devices. Here, we report the synthesis and optoelectronic properties of highly conductive (≤ 1180 S cm -1 ) poly(3,4-ethylenedioxythiophene) (PEDOT) films prepared by vapor phase polymerization (VPP). We focus on their application in ITO-free OLEDs as a patternable organic anode material. We describe devices fabricated on glass and flexible plastic substrates with efficiencies (16.8 and 9.8 lm W PEDOT is an especially promising organic electrode material. Though insoluble in all common solvents, PEDOT films exhibit a number of desirable properties in the oxidized state, including high conductivity, good stability, and high thin-film transparency. [6,7] It is possible to circumvent the low solubility of PEDOT using a water-soluble polyelectrolyte such as poly(styrene sulfonic acid) (PSSA) during polymerization in water, yielding a PEDOT-PSS aqueous composite with good film-forming properties. [8,9] However, the conductivity of a PEDOT-PSS film is typically no more than ca. 10 S cm -1 , well below the level typical of ITO (ca. 4000 S cm -1 ). Researchers have explored several methods for raising the conductivity, including the addition of a range of secondary dopants.