Abstract
Spider silks represent stretchable and contractible fibers with high toughness. Those tough fibers with stretchability and contractibility are attractive as energy absorption materials, and they are needed for wearable applications, artificial muscles, and soft robotics. Although carbon-based materials and poly(vinyl alcohol) (PVA) composite fibers exhibit high toughness, they are still limited in low extensibility and an inability to operate in the wet-state condition. Herein, we report stretchable and contractible fiber with toughness that is inspired by the structure of spider silk. The bioinspired tough fiber provides 495 J/g of gravimetric toughness, which exceeds 165 J/g of spider silk. Besides, the tough fiber was reversibly stretched to ∼80% strain without damage. This toughness and stretchability are realized by hybridization of aligned graphene oxide/multiwalled carbon nanotubes in a polyurethane matrix as elastic amorphous regions and β-sheet segments of spider silk. Interestingly, the bioinspired tough fiber contracted up to 60% in response to water and humidity similar to supercontraction of the spider silk. It exhibited 610 kJ/m3 of contractile energy density, which is higher than previously reported moisture driven actuators. Therefore, this stretchable and contractible tough fiber could be utilized as an artificial muscle in soft robotics and wearable devices.