Polymeric dielectrics with high dielectric permittivity (ɛ′) and low loss have momentous applications in energy storage devices. In this study, to concurrently improve the ɛ′ and restrain the loss of original Zn (Zinc)/poly(vinylidene fluoride, PVDF), the core@double‐shell structured Zn@ZnO(zinc oxide)@PS(polystyrene) particles were prepared and composited with the PVDF. The impacts of the dual shells on the dielectric properties and polarization mechanism of composites were explored by fitting the experimental data with a Havriliak–Negami (H–N) equation. The Zn@ZnO@PS/PVDF exhibit remarkably higher ɛ′ in comparison to the raw Zn and Zn@ZnO fillers owing to the induced multiple polarizations originating from the combined contributions of the α relaxation of PVDF, slow interparticle polarization and fast intraparticle polarization. More importantly, the ɛ′ of the composites remarkably increases with the PS shell’ thickness, while the loss is still kept at rather low levels owing to the PS shell’ barrier effect on long‐range charges migration. So, the introduction of the PS shell synchronously promotes both the interparticle and intraparticle polarizations in the Zn@ZnO@PS/PVDF composites toward enhanced dielectric properties. The developed strategy opens a novel path to the design and fabrication of polymer composites with desirable dielectric performances for applications in electronics and electrical industry.

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In order to synchronously improve dielectric permittivity (ε 0 ), breakdown strength (E b ), and thermal conductivity (TC) while inhibiting dissipation factor (tan δ) of raw Zn (Zinc)/PVDF (poly[vinylidene fluoride]) composites, two kinds of core-shell structured particles of Zn@ZnO (zinc oxide) and Zn@ZnO@PS (polystyrene) were synthesized by high-temperature oxidation followed by suspension polymerization, then they were composited with PVDF to elaborately generate morphology-controllable high-ε 0 but low loss, and high TC composites. The results confirm that both the Zn@ZnO/PVDF and Zn@ZnO@PS/PVDF composites show markedly improved ε 0 , suppressed tan δ and conductivity over the original Zn/PVDF because of the induced multiple polarizations in the Zn@ZnO and Zn@ZnO@PS configurations and the barrier effect of constructed shells on direct contact of Zn particles. The second organic PS shell inhibits the loss and conductivity due to its high-electrical resistivity, and further boosts the E b and TC of the composites owing to enhanced interfacial compatibility between the Zn@ZnO and PVDF, which lessens the local electric field distortion and concentration, and therefore, promotes phonon transport across the interfaces through suppressing the thermal interfacial resistance. The prepared Zn@ZnO@PS/PVDF with a high E b and ε 0 but low tan δ, as well as enhanced TC, exhibit appealing potential applications in microelectronic devices and power equipment.

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