The
actuation and energy-harvesting performance of dielectric elastomers
are strongly related to their intrinsic electrical and mechanical
properties. For future resilient smart transducers, a fast actuation
response, efficient energy-harvesting performance, and mechanical
robustness are key requirements. In this work, we demonstrate that
poly(styrene-butadiene-styrene) (SBS) can be converted into a self-healing
dielectric elastomer with high permittivity and low dielectric loss,
which can be deformed to large mechanical strains; these are key requirements
for actuation and energy-harvesting applications. Using a one-step
click reaction at room temperature for 20 min, methyl-3-mercaptopropionate
(M3M) was grafted to SBS and reached 95.2% of grafting ratios. The
resultant M3M–SBS can be deformed to a high mechanical strain
of 1000%, with a relative permittivity of εr = 7.5
and a low tan δ = 0.03. When used in a dielectric actuator,
it can provide 9.2% strain at an electric field of 39.5 MV m–1 and can also generate an energy density of 11 mJ g–1 from energy harvesting. After being subjected to mechanical damage,
the self-healed elastomer can recover 44% of its breakdown strength
during energy harvesting. This work demonstrates a facile route to
produce self-healing, high permittivity, and low dielectric loss elastomers
for both actuation and energy harvesting, which is applicable to a
wide range of diene elastomer systems.