High permittivity and breakdown strength are desired to improve the energy storage density of dielectric materials based on reinforced polymer composites. This article presents the synthesis of polythiophene-encapsulated BaTiO3 (BTO-PTh) nanoparticles via an in situ Cu(II)-catalyzed chemical oxidative polymerization of thiophene monomer on hydrothermally obtained tetragonal BTO nanocrystals. The formed core–shell-type BTO-PTh nanoparticles exhibit excellent dielectric properties with high permittivity (25.2) and low loss (0.04) at high frequency (106 Hz). A thick PTh encapsulation layer on the surface of the BTO nanoparticles improves their breakdown strength from 47 to 144 kV/mm and the energy storage density from 0.32 to 2.48 J/cm3. A 7.75-fold increase in the energy storage density of the BTO-PTh nanoparticles is attributed to simultaneously high permittivity and breakdown strength, which are excellent for potential energy storage applications.
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