▎ 摘　　要

The flexible metacomposites with tunable negative permittivity have great potential in wearable cloaks, stretchable sensors, and thin-film capacitors, etc. In this paper, the flexible graphene/polydimethylsiloxane (GR/PDMS) metacomposites with tunable negative permittivity were prepared by an in situ polymerization method. The ac conductivity behavior, dielectric property, and impedance performance of the resulting composites with different graphene mass ratios (0-4 wt %) were studied. With the increase of graphene, the conductive mechanism of the resulting composites changed from hopping conduction to electron conduction, along with the change of microstructure. When graphene content in the composites came up to 3 wt %, the negative permittivity conforming to Drude model was observed. Further investigation revealed that there is a corresponding relationship between the permittivity and the reactance. It is demonstrated that the inductive character is responsible for the negative permittivity, while the capacitive character results in the positive permittivity.