The development of waterproof ionogels
with high stretchability
and fast self-healing performance is essential for stretchable ionic
conductors in sophisticated skin-inspired wearable sensors but can
be rarely met in one material. Herein, a semicrystalline fluorinated
copolymer ionogel (SFCI) with extremely high stretchability, underwater
stability, and fast self-healability was fabricated, among which hydrophobic
ionic liquids ([BMIM][TFSI]) were selectively enriched in fluoroacrylate
segment domains of the fluorinated copolymer matrix through unique
ion–dipole interactions. Benefiting from the reversible ion–dipole
interactions between the [BMIM][TFSI] and fluoroacrylate segment domains
as well as the physical cross-linking effects of semicrystalline oligoethylene
glycol domains, the SFCI exhibited ultrastretchability (>6000%),
fast
room-temperature self-healability (>96% healing efficiency after
cutting
and self-healing for 30 min), and outstanding elasticity. In addition,
the representative SFCI also exhibited high-temperature tolerance
up to 300 °C, antifreezing performance as low as −35 °C,
and high transparency (>93% visible-light transmittance). As a
result,
the as-obtained SFCI can readily be used as a highly stretchable ionic
conductor in skin-inspired wearable sensors with waterproof performance
for real-time detecting physiological human activities. These attractive
features illustrate that the developed ultrastretchable and rapidly
self-healable ionogels with unique waterproofness are promising candidates
especially for sophisticated wearable strain sensing applications
in complex and extreme environments.