Dielectric elastomers generate muscle-like electroactive actuation, which is applicable in soft machines, medical devices, etc. However, the actuation strain and energy density of most dielectric elastomers, in the absence of prestretch, have long been limited to ∼20% and ∼10 kJ m-3, respectively. Here, we report a dielectric elastomer with ZrO2 nanoparticles confined in nanodomains, which achieves an actuation strain >100% and an energy density of ∼150 kJ m-3 without prestretch. We decorate the surface of each nanoparticle with a layer of a diblock oligomer, poly(acrylic acid-b-styrene). The surface-decorated nanoparticles coassemble with a triblock copolymer elastomer, poly(styrene-b-(2-ethylhexyl acrylate)-b-styrene) during cosolvent casting. Consequently, the nanoparticles are confined in the polystyrene nanodomains, which results in a dielectric elastomer nanocomposite with a low modulus, high breakdown strength, and intense strain-hardening behavior. During the actuation, the nanocomposite avoids the snap-through instability that most elastomers would suffer and achieves a superior actuation performance.
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