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Outside of the active device layers, there are a variety of requisite functional layers in flexible organic electronic devices. Whether the application is in displays, lighting, integrated circuits, or photovoltaics, there are materials challenges in implementing flexible and/or organic devices into practical applications. We highlight two topics that are common to most flexible electronic technologies. First, we describe the difficulty in developing suitable permeation barriers on polymer substrates, the approaches being taken to solve this problem, and their current status. Second, we highlight the limited mechanical ruggedness of brittle inorganic films and present approaches for improving overall device flexibility.