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This article provides an overview of the present state-of-the-art pertaining to polymer capacitor dielectrics appropriate for high electrostatic energy density applications. The challenges and opportunities surrounding capacitor materials development/discovery in a practical context are reviewed. It is pointed out that several hierarchical considerations ranging from dielectric, electronic, morphological, processing, reliability and electrical characteristics need to be confronted and addressed adequately before one can progress from “standard” materials (such as biaxially oriented polypropylene) toward next generation materials. Nevertheless, it is argued that the prospects for systematic approaches toward polymer dielectrics discovery appear to be strong, especially given recent successes and evidence that a cooperative computation-synthesis-processing-characterization paradigm can bear fruit. It is hoped that this …