Strong, tough and anisotropic bioinspired hydrogels.

Soft materials are widely used in tissue engineering, soft robots, wearable electronics, However, it remains a challenge to fabricate soft materials, such as hydrogels, with both high strength and toughness that are comparable to biological tissues. Inspired by the anisotropic structure of biological tissues, a novel solvent-exchange-assisted wet-stretching strategy is proposed to prepare anisotropic polyvinyl alcohol (PVA) hydrogels by tuning the macromolecular chain movement and optimizing the polymer network. The reinforcing and toughening mechanisms are found to be "macromolecule crystallization and nanofibril formation". These hydrogels exhibit excellent mechanical properties, such as extremely high fracture stress (12.8 ± 0.7 MPa) and fracture strain (1719 ± 77%), excellent modulus (4.51 ± 0.76 MPa), high work of fracture (134.47 ± 9.29 MJ m), and fracture toughness (305.04 kJ m) compared with other strong hydrogels and even natural tendons. In addition, excellent conductivity, strain sensing capability, water retention, freezing resistance, swelling resistance, and biocompatibility can also be achieved. This work provides a new and effective method to fabricate multifunctional anisotropic hydrogels with high tunable strength and toughness with potential applications in the fields of regenerative medicine, flexible sensors, and soft robotics.