General Principle for Fabricating Natural Globular Protein-Based Double-Network Hydrogels with Integrated Highly Mechanical Properties and Surface Adhesion on Solid Surfaces

Developing functional hybrids of globular proteins and synthetic polymers into multipurpose tough hydrogels remains challenging. Here, we propose a new strategy combining double-network and protein misfolding concepts to create diverse protein–polymer double-network (DN) hydrogels with both high bulk and interfacial toughness. The method integrates an intrinsic heat-induced protein denaturation/aggregation feature and a double-network concept, which produces different bovine serum albumin (BSA)-based DN hydrogels with hybrid physical–chemical cross-linking or fully physical cross-linking to achieve a high modulus of 252–1199 kPa, high strength of 0.24–0.48 MPa, high fracture energy of 3.56–16.88 MJ/m3, high extensibility of 7.7–79.9 mm/mm, fast self-recovery (stiffness/toughness recovery of 94/80% after heat treatment at 80 °C for 30 min), and strong surface adhesion to various nonporous solid surfaces (interfacial toughness of 1176–2827 J/m2). Such tough and adhesive protein–polymer hydrogels have great potential for different applications, such as artificial soft tissues, flexible electronics, and wearable devices.