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Heat accumulation has emerged as a critical issue that affects the performance and reliability of modern electronic devices in their evolving toward miniaturization, high power density and high integration. The application of thermal interface materials (TIMs) as a thermal management strategy is commonly employed to tackle this problem. Herein, we report the development and characterization of highly thermally conductive but electrically insulating Cu@Al 2 O 3 /epoxy composites. Stemming from the excellent thermal conductivity of Cu, the Cu@Al 2 O 3 /epoxy composites exhibit thermal conductivity of 1.32 W/m·K at 10 vol% filler content, which is nearly 7 times higher than that of the epoxy resin. Simultaneously, the Cu@Al 2 O 3 /epoxy composites still retain a high electrical resistivity of 2.3 × 1013 Ω·cm, which is 6 orders of magnitude greater than that of Cu/epoxy composites without Al 2 O 3 barrier layers, because the dense nanoscale insulating Al 2 O 3 shell effectively inhibits the electron transfer. In addition, the Cu@Al 2 O 3 /epoxy composites possess lower dielectric constant and dielectric loss, and better mechanical properties than those of Cu/epoxy composites. [Display omitted] • Core-shell Cu@Al 2 O 3 particles were rationally designed and prepared by a simple and scalable solution-based process. • Cu@Al 2 O 3 /epoxy composites were fabricated as thermal interface materials for thermal management application. • Enhanced thermal conductivity and high electrical insulation was achieved by Cu@Al 2 O 3 /epoxy at a low filler content. • Cu@Al 2 O 3 /epoxy composites possess better dielectric and mechanical performances than those of Cu/epoxy composites. [ABSTRACT FROM AUTHOR]

[Display omitted] • Core-shell structured Cu@BaTiO 3 particles were prepared. • Cu@BaTiO 3 /epoxy composites were fabricated as thermal interface materials. • The thermal conductivity was enhanced and high electrical insulation was retained for Cu@BaTiO 3 /epoxy composites. The application of polymer for thermal interface materials is limited by its low thermal conductivity. In this work, barium titanate coated Cu core–shell particles were prepared and then employed as thermal conductive fillers to reinforce epoxy matrix. The results indicate that thermal conductivity of the Cu@BaTiO 3 /epoxy composites reaches 1.09 W m-1K−1 at 10 vol% loading, achieving 580% elevation on neat epoxy matrix. Meanwhile, the composites retain high electrical insulation (7.90 × 1013 Ω·cm) due to the existence of insulative BaTiO 3 layer on Cu surface. This study will provide a novel insight of the design of functionalized core–shell thermal conductive fillers and construction of high-performance thermal interface materials. [ABSTRACT FROM AUTHOR]