Soft robotics focuses on mimicking natural systems to produce dexterous motion. Dielectric elastomer actuators (DEAs) are an attractive option due to their large strains, high efficiencies, lightweight design, and integrability, but require high electric fields. Conventional approaches to improve DEA performance by incorporating solid fillers in the polymer matrices can increase the dielectric constant but to the detriment of mechanical properties. In the present work, we draw inspiration from soft and deformable human skin, enabled by its unique structure, which consists of a fluid-filled membrane, to create self-enclosed liquid filler (SELF)–polymer composites by mixing an ionic liquid into the elastomeric matrix. Unlike hydrogels and ionogels, the SELF–polymer composites are made from immiscible liquid fillers, selected based on interfacial interaction with the elastomer matrix, and exist as dispersed globular phases. This combination of structure and filler selection unlocks synergetic improvements in electromechanical propertiesdoubling of dielectric constant, 100 times decrease in Young’s modulus, and ∼5 times increase in stretchability. These composites show superior thermal stability to volatile losses, combined with excellent transparency. These ultrasoft high-k composites enable a significant improvement in the actuation performance of DEAslongitudinal strain (5 times) and areal strain (8 times)at low applied nominal electric fields (4 V/μm). They also enable high-sensitivity capacitive pressure sensors without the need of miniaturization and microstructuring. This class of self-enclosed ionic liquid polymer composites could impact the areas of soft robotics, shape morphing, flexible electronics, and optoelectronics.

Ionic liquid incorporation into Diels–Alder adduct based healable polymers drastically reduces their healing temperature and improves their mechanical and dielectric properties.

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