High-quality electrophotographic applications demand a photoreceptor drum that is “perfect” in many aspects, such as being defect-free—almost to the submicrometer level, environmentally insensitive, and possessing a well-defined photosensitivity that matches the electrophotographic rendering process. The surface quality of the substrate strongly influences the quality of the critical charge-generation layer. Every minute defect of the substrate surface is magnified in that layer. Almost always, a substrate surface-smoothing layer is required. This work describes the development of aqueous, environmentally green compositions for thick, uniform, defect-free, transparent, and conductive surface-smoothing layers.