Silicone rubber (SR)/polyolefin elastomer (POE) blends containing ionic liquids modified with carbon blacks (CB-IL) and multi-walled carbon nanotubes (CNT-IL) were prepared by melt-blending and hot pressing. SR/POE/CB-IL and SR/POE/CB-CNT-IL composites showed co-continuous structural morphologies. The cation–π interactions between ILs and CNTs were stronger than those between ILs and CBs due to the large length and high surface area of CNTs, which promoted better dispersion of carbon fillers. SR/POE/CB-CNT-IL composites showed higher EMI SE than SR/POE/CB-IL composites containing identical filler contents because the CNTs with larger aspect ratios helped form more electrically-conductive networks.
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