ABSTRACTOrganically modified dielectric filler nanoparticles with core–shell structures have received widespread attention when designing composites with excellent dielectric properties. Herein, the core–shell structured BaTiO3@polyethylene (BT@PE) nanoparticles were prepared and the models of BT@PE filled low‐density polyethylene (LDPE) composites were constructed. The interaction modulated nanoparticle dispersion structure and the effect of the core–shell structured BT@PE on the polarization and breakdown of the composites were studied by molecular dynamics (MD) simulations and finite element analysis (FEA). The results show that BT@PE modulated the interactions between particles, formed a well‐dispersed structure in the LDPE matrix, and optimized the electric field distribution inside the composites. Moreover, due to the existence of microscopic transition layer, the core–shell structured BT@PE increased the interfacial polarization while suppressed the electric field distortion. BT@PE nanoparticles simultaneously enhanced the dielectric constant and breakdown strength of the composites.
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