Epsilon‐negative materials with lower percolation threshold derived from segregated structures

Epsilon‐negative materials (ENM) at radio frequency, usually designed based on percolation theory, recently drew much attention because of their potential applications in capacitors, transistors, and antennas. However, randomly distributed conductive functional materials cannot achieve directional long‐range electron transportation within the material, resulting in decreased utilization efficiency. The morphology design of the substrate material can change the distribution state and electron transfer pathway of conductive fillers. By controlling the size of the polystyrene (PS) and the content of multi‐walled carbon nanotubes (MWCNTs), PS/MWCNTs composites with random structures and segregated structures were designed, both of which exhibited negative permittivity with increasing MWCNTs content. Further investigation revealed that negative permittivity behavior is due to the establishment of the conductive network and the plasma oscillation of free electrons. Moreover, components with segregated structures have lower percolation thresholds, as directional electron transport is achieved and conductive fillers are efficiently utilized. This work provides a new method for guiding the electron transport pathway and effectively changing the distribution state of conductive fillers in ENM. Highlights Negative permittivity is achieved by plasma oscillation at radio frequency. The segregated structure leads to a decrease in the percolation threshold. Epsilon‐negative materials have good prospects in inductive components. Epsilon‐negative materials based on segregated structure and random structure.