Robust Multiscale-Oriented Thermoresponsive Fibrous Hydrogels with Rapid Self-Recovery and Ultrafast Response Underwater

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.