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 propertiesdoubling 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 DEAslongitudinal
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.