Ionic polymer-metal composites (IPMC) are devices composed of metallic electrodes and an ionomeric polymer membrane in a “sandwich” architecture and. Their main property is electromechanical actuation or sensing based on the movement of ions. Metallic electrodes are commonly used for their high electrical conductivity, malleability, and chemical resistance. However, the high cost of noble metals, such as platinum, long manufacturing time, and fatigue failure limit their application. Therefore, the replacement of metallic electrodes with Conductive Elastomeric Nanocomposites (CENs) was evaluated to reduce the costs and complexity of manufacturing the device and increase its working life. In this work, carbon nanotubes were used as the conductive fillers. The dispersion to achieve high electrical conductivity was carried out directly in the synthetic or natural polyisoprene rubber latex assisted by surfactant and high-power sonication. To improve the adhesion between the elastomeric electrode and the ionic membrane (Nafion), plasma treatment with atmospheric air was applied as a surface modifier. This treatment improved the hydrophilicity and adhesion of the rubbers by forming oxygenated groups and increasing the surface nanoroughness. In this way, ionomeric polymer-polymer composite (IP²C) devices were fabricated using Nafion and plasma-modified CENs, this type of electrode is unprecedented in the literature for this application. These devices showed displacement and strain sensing capacity at levels close to the conventional IPMC in all tested frequency ranges and applied accelerations. Notably, the IP²C obtained better resolution at low frequencies than the control.