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Dielectric materials with high thermal conductivity and outstanding dielectric properties are highly desirable for advanced electronics. However, simultaneous integration of those superior properties for a material remains a daunting challenge. Here, a multifunctional epoxy composite is fulfilled by incorporation of boron nitride nanosheets (BNNSs) and mesoporous silica coated multi-walled carbon nanotubes (MWCNTs@mSiO2). Owing to the effective establishment of continuous thermal conductive network, the obtained BNNSs/MWCNTs@mSiO2/epoxy composite exhibits a high thermal conductivity of 0.68 W m−1 K−1, which is 187% higher than that of epoxy matrix. In addition, the introducing of mesoporous silica dielectric layer can screen charge movement to shut off leakage current between MWCNTs, which imparts BNNSs/MWCNTs@mSiO2/epoxy composite with high dielectric constant (8.10) and low dielectric loss (<0.01) simultaneously. It is believed that the BNNSs/MWCNTs@mSiO2/epoxy composites with admirable features have potential applications in modern electronics. [ABSTRACT FROM AUTHOR]