Super Strong and Tough PVA Hydrogel Fibers Based on an Ordered‐to‐Disordered Structural Construction Strategy Targeting Artificial Ligaments

Abstract Hydrogels with high strength, high modulus, and high toughness have great application potential in the field of artificial human load‐bearing tissues, but the preparation of materials with the above high performance is still a huge challenge. In this paper, a structural construction strategy of ordered‐to‐disordered (OTD) transition is proposed to obtain hydrogel fibers with high strength, high modulus, and high toughness. The structural construction strategy of OTD refers to the ordered‐to‐disordered transition of molecular segments in PVA polymer fibers through swelling and subsequent salting‐out treatment, while still maintaining the general order of the entire polymer chain. PVA molecular chain crystallites provide physical crosslinking to stabilize the structure. The results show that the elongation at break of the hydrogel fiber can reach 257%). The strength reaches 190.04 MPa, which is more than 4 times higher than that of human ligaments. The modulus reaches 137.31 MPa, which perfectly matches the human ligaments, and the toughness can reach 100.61 MJ m −3 . In addition, it has stable mechanical properties in liquid environment and excellent biocompatibility, which has great application potential in the field of artificial ligaments. This OTD structural construction strategy provides a facile approach to achieving hydrogel fibers with desired mechanical properties.