▎ 摘　　要

Composites with negative permittivity have drawn much attentions for novel capacitance design and electromagnetic shielding applications. Herein, polyphenylene sulfide (PPS) matrix composites filled with graphene were prepared by hot-pressing for tailorable negative permittivity media. Electrical percolation occurred as graphene content increasing and the conduction mechanism changed into free electron model. Graphene/PPS composites with tailorable negative permittivity properties were realized, resulting from the plasmonic oscillation of free electrons in composites exceeding percolation threshold. The regulation mechanism of negative permittivity in this random composite was clarified, and the obtained tailorable negative permittivity media could be novel candidates for various electromagnetic applications. (C) 2019 Elsevier B.V. All rights reserved.