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To meet the demand of emerging devices for highfrequency dielectric performances, we proposed semiconductor polyaniline in situ modified rGO nanosheets to keep the dielectric constant stable at high frequencies. The π−π interface interaction between rGO and semiconductor polyaniline was found to block the migration of electrons, redistributing the delocalized electrons of rGO and leading to a reduction in relaxation time and a delay in the dielectric relaxation at higher frequencies. This mechanism gave the dielectric materials a stable dielectric constant at high frequencies. The dielectric relaxation time was reduced from 2.75 × 10 −8 to 5.68 × 10 −10 at a filler load of 10 wt %. The dielectric constant only decreased by 19% from 100 to 1 × 10 8 Hz. For the same range, unmodified rGO showed an 85% decrease. This mechanism could also further increase the dielectric constant and decrease the dielectric loss. This has a great potential for emerging high-frequency devices (DC/DC converter, sensors, energy harvesters, etc.).

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