Al@SiO(2) Core–Shell Fillers Enhance Dielectric Properties of Silicone Composites

[Image: see text] Over the past decade, there has been significant interest in polysiloxane-based dielectric elastomers as promising soft electroactive materials. Nevertheless, the natural low permittivity of polydimethylsiloxane has limited its practical applications. In this study, we have developed silicone rubber/Al@SiO(2) composites with a high dielectric constant, low dielectric loss, and high electrical breakdown strength by controlling the shell layer thickness and the content of the core–shell filler. We also investigated the dielectric behavior of the composites. The use of core–shell fillers has increased the Maxwell–Wagner–Sillars (MWS) relaxation process while reducing the dielectric loss of direct current conductance in silicone rubber composites. Moreover, the temperature dependence of the MWS relaxation time in the composites follows the Arrhenius equation. This strategy of increasing the permittivity of silicone composites through core–shell structural fillers can inspire the preparation of other high dielectric constant composites.