Hydrogels
with ultrafast response to environmental stimuli, possessing
robust structural integrity and rapid self-recovery, have been considered
as promising platforms for numerous applications, for example, in
biomimetic materials and nanomedicine. Inspired by the bundled fibrous
structure of actin, we developed a robust and ultrafast thermoresponsive
fibrous hydrogel (TFH) by fully utilizing the weak noncovalent bonds
and strong covalently cross-linked semiflexible electrospun fibrous
nets. The TFH exhibits an ultrafast response (within 10 s), rapid
self-recovery rate (74% within 10 s), tunable tensile strength (3–380
kPa), and high toughness (∼1560 J/m2) toward temperature.
A multiscale orientation is considered to play a key role in the excellent
mechanical properties at the fibrous mesh, fiber, and molecular scales.
Furthermore, to take advantage of this TFH adequately, a novel kind
of noodle-like hydrogel for thermo-controlled protein sorption based
on the TFH is prepared, which exhibits high stability and ultrafast
sorption properties. The bioinspired platforms hold promise as artificial
skins and “smart” sorption membrane carriers, which
provide a unique bioactive environment for tissue engineering and
nanomedicine.