Artificial Spider Silk with Buckled Sheath by Nano‐Pulley Combing

The axial orientation of molecular chains always results in an increase in fiber strength and a decrease in toughness. Here, taking inspiration from the skin structure, artificial spider silk with a buckled sheath-core structure is developed, with mechanical strength and toughness reaching 1.61 GPa and 466 MJ m-3 , respectively, exceeding those of Caerostris darwini silk. The buckled structure is achieved by nano-pulley combing of polyrotaxane hydrogel fibers through cyclic stretch-release training, which exhibits axial alignment of the polymer chains in the fiber core and buckling in the fiber sheath. The artificial spider silk also exhibits excellent supercontraction behavior, achieving a work capacity of 1.89 kJ kg-1 , and an actuation stroke of 82%. This work provides a new strategy for designing high-performance and intelligent fiber materials.