The growing interest toward biocompatible and bioinspired materials is boosting the investigation and the engineering of natural products as active components in electronic devices. The human pigment melanin, and particularly its subgroup composed by the eumelanins, the black-brown pigments derived from the oxidative polymerization of L-3,4-dihydroxyiphenylalanine (l-DOPA) via 5,6-dihydroxy-indole intermediates are increasingly emerging as valuable candidates for organic (bio)electronics applications. Capitalizing on a recently developed protocol to prepare high quality eumelanin coatings, this paper reports herein the design and the integration of standard commercial poly(3,4-ethylenedioxythiophene) with the poly(styrenesulfonate) (PEDOT:PSS) with eumelanin pigment. The new blend has made it possible to obtain a water stable quite transparent thin film, able to operate as an electrode for organic devices, complementing the PEDOT:PSS conductivity with the peculiar eumelanin properties, including adhesion, water stability, and ionic–electronic conductivity. As proof of concept, an unprecedented indium tin oxide-free organic light emitting diode implementing an eumelanin–PEDOT layer as the anode is fabricated and characterized. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

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