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Conductive polymer composites require high conductive filler loadings to achieve relatively ideal electromagnetic interference (EMI) shielding performance, which brings problems such as heavy weight and poor processability and ultimately limits their application in the aerospace field. To solve the above problems and realize the preparation of excellent EMI shielding composites with low filler loadings, a bipolar pulsed electric field-induced graphene nanoplatelets (GNPs) alignment method is proposed in this paper to improve the electrical conductivity and EMI shielding performance. The orientation and alignment of GNPs in the matrix were characterized by x-ray diffraction and scanning electron microscopy, and the results showed that GNPs formed a conductive network. The electrical conductivity of the composite material in the X-band was measured, and the results showed that the bipolar pulsed electric field could significantly improve the electrical conductivity of the composite material; the improvement percentage reached 100%–300% under the five filler loadings. In addition, the EMI shielding effectiveness of the composite material in the X-band was tested. The results showed that the EMI shielding effectiveness of the composite material with a mass fraction of 14% increased from 16.48–15.86 dB to 21.37–20.99 dB with the action of the bipolar pulsed electric field, and the improvement percentage was 32%. This is the first study on improving the EMI shielding performance of composite materials by applying a bipolar pulsed electric field, and it provides an effective method to prepare EMI shielding composites with low filler loadings. [ABSTRACT FROM AUTHOR]