Flexible and lightweight graphene nanosheet (GN)/waterborne polyurethane (WPU) composites which exhibit high electrical conductivity and electromagnetic shielding performance were prepared. Covalently modifying GNs with aminoethyl methacrylate (AEMA; AEMA-GNs) through free radical polymerization effectively inhibited the restacking and aggregation of the GNs because of the -NH3(+) functional groups grafted on the AEMA-GNs. Moreover, the AEMA-GNs exhibited high compatibility with a WPU matrix with grafted sulfonated functional groups because of the electrostatic attraction, which caused the AEMA-GNs to homogeneously disperse in the WPU matrix. This homogeneous distribution enabled the GNs to form electrically conductive networks. Furthermore, AEMA-GNs with different amounts of AEMA segments were introduced into the WPU matrix, and the effects of the surface chemistry of the GNs on the electrical conductivity and EMI shielding performance of composites were investigated. AEMA-GN/WPU composites with a GN loading of 5 vol % exhibited remarkable electrical conductivity (approximately 43.64 S/m) and EMI shielding effectiveness (38 dB) over the frequency of 8.2 to 12.4 GHz.
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