摘要:SummaryDielectric capacitors with higher working voltage and power density are favorable candidates for renewable energy systems and pulsed power applications. A polymer with high breakdown strength, low dielectric loss, great scalability, and reliability is a preferred dielectric material for dielectric capacitors. However, their low dielectric constant limits the polymer to achieve satisfying energy density. Therefore, great efforts have been made to get high-energy-density polymer dielectrics. By compositional and structural tailoring, the synergic integrations of the multiple components and optimized structural design effectively improved the energy storage properties. This review presents an overview of recent advancements in the field of high-energy-density polymer dielectrics via compositional and structural tailoring. The surface/interfacial engineering conducted on both microscale and macroscale for polymer dielectrics is the focus of this review. Challenges and the promising opportunities for the development of polymer dielectrics for capacitive energy storage applications are presented at the end of this review.Graphical abstractDisplay OmittedHighlights•A detailed summary of the state-of-the-art polymer dielectrics•The comparison of polymer nanocomposites with 0D, 1D, and 2D nanofillers•Analyzing highUepolymer dielectrics via compositional and structural tailoring•Summary of micro- or macro-surface and interface engineeringElectrochemical energy storage; Energy materials; Materials science; Polymers