摘要： For polymer-based nanocomposites, designing the nanostructures of fillers, their distribution inside matrix as well as interfaces with the polymer is of crucial importance to achieve high dielectric performances. One-dimensional semiconductor Bi2S3 nanorods coated with homogeneous SiO2 and polydopamine (PDA) double shell layers were imported into the poly(vinylidene fluoride) (PVDF) with parallel arrangement via uniaxial stretching to form Bi2S3@SiO2@PDA/PVDF nanocomposite. The dielectric performances of oriented Bi2S3@SiO2@PDA/PVDF were studied in comparison with its counterparts employing Bi2S3 fillers without shell layers or alignment. A microcapacitor model was used to accurately estimate the dielectric constant along perpendicular direction. Coating conductive Bi2S3 nanorods with insulating SiO2@PDA double layer remarkably reduces the dielectric loss of the nanocomposite, while alignment of one-dimensional Bi2S3@SiO2@PDA nanorods endows electrical properties anisotropy, which was understood from J-V curves measured along two directions and moreover, via three-dimensional finite element analysis, unambiguously revealing the effects of aligned core-shell structured fillers on local electric field and current density distribution. This study provides a promising and facile approach for designing high performance dielectrics.