This paper presents a novel strategy to modify the surface chemistry of barium titanate (BaTiO3, BT) with a bimodal population of oligothiophene polymer brushes using step-by-step reversible addition fragmentation chain transfer (RAFT) polymerization. Compared with a previous strategy based On monornodal surface-tethered brushes, these hybrid nanopartides, BaTiO3 coated with-bimodal oligothiophene polymer brushes, demoristrate extremely good dispersion behaviors as dielectric nariofillers in a matrix of oligothiophene polymers. These nanodielectric composites exhibit greatly improved dielectric performance and maintain linear displacement-polarization (D-E) profiles under high applied electric fields. This promising bimodal strategy,could be generalized to a variety of nanoparticles for the development of novel dielectric nanocomposite systems: