One Stone, Two Birds: Spidroin‐Inspired Nanogels for High‐Performance Fibers and Photothermal Actuators

Abstract The exciting development of hydrogels makes it a promising candidate to be applied in various fields. However, it remains a great challenge to store the precursors of hydrogels and to process them after gelation, like synthetic polymer materials. Herein, spidroin‐inspired novel nanogels with extraordinary processability, which can be spun into fibers via direct drawing and fabricated into thermal actuators easily after gelation are prepared. These soluble and spinnable nanogels are composed of a liquid metal core and a poly (acrylic acid) (PAA) shell and are entangled with each other. The as fabricated nanogels and diluted dope solution can be stored >1 month. The as‐spun nanogel fibers with hierarchical structures achiev extraordinary mechanical properties (tensile stress of 575 MPa, toughness of 381 MJ m −3 ) and supercontraction at 60% RH. Besides, a photothermal actuator is prepared by coating the nanogels on a polyethylene substrate with a commercial shading ink, and the as‐prepared actuator shows a rapid response to near‐infrared light as well as a fast recovery. Molecular dynamics simulation reveals a possible working mechanism of the actuator. This study provides a new strategy to prepare processable nanogels with broad application prospects for smart textiles and soft robots.