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With the continuous advancement of electronic devices, there is an urgent need for advanced thermal interface materials (TIMs) to prevent high-power density electronics from overheating. The orderly arrangement of thermally conductive fillers in TIMs plays a crucial role in enhancing thermal conduction along preferred directions. However, it is challenging to control the orientation of the fillers, especially for two-dimensional fillers. In this study, graphene nanoplates (GNPs) were co-planarly arranged in polyvinyl alcohol (PVA) using a rotating magnetic field, which significantly increased the thermal conductivity of the composites. The coplanar vertically aligned GNPs/PVA (CVGNPs/PVA) exhibited a through-plane thermal conductivity of 11.78 W m−1 K−1, which is about 10 times higher than that of the composites with disorderly distributed GNPs (1.14 W m−1 K−1). The rotating magnetic field facilitated the alignment of GNPs and increased face-to-face contact between adjacent GNPs, which significantly boosted the through-plane thermal conductivity of the composite. The compressive modulus of the CVGNPs/PVA composites was only 1.06 MPa, and it helped to reduce the thermal interface resistance to 49 mm2 K W−1. These results offer a novel approach for preparing excellent TIMs that could be used in various applications. GNPs are oriented more compactly and orderly in PVA by using the rotating magnetic field, resulting in a densified thermal conductive paths and higher thermal conductivity of the composite. [Display omitted] [ABSTRACT FROM AUTHOR]