One-Pot Fabrication of Supramolecular Synthetic Protein Hydrogel with Tissue-like Integrated Dynamic Features

Protein-incorporated soft networks have received remarkable attention during the past several years. They possess desirable properties similar to native tissues and organs and exhibit unique advantages in applications. However, fabrication of protein-based hydrogels usually suffers from complex protein mutation and modification or chemical synthesis, which limited the scale and yield of production. Meanwhile, the lack of rationally designed noncovalent interactions in networks may result in a deficiency of the dynamic features of materials. Therefore, a highly efficient method is needed to include supramolecular interactions into protein hydrogel to generate a highly dynamic hydrogel possessing integrated tissue-like properties. Here, we report the design and construction of native protein-based supramolecular synthetic protein hydrogels through a simple and efficient one-pot polymerization of acrylamide and ligand monomers in the presence of a ligand-binding protein. The supramolecular interactions in the network yield integrated dynamic properties, including remarkable stretchability over 10,000% of their original length, ultrafast self-healing abilities within 3–4 s, tissue-like fast stress relaxation, satisfactory ability of adhesion to different living and nonliving substrates, injectability, and high biocompatibility. Furthermore, this material demonstrated potential as a biosensor to monitor small finger movements. This strategy provides a new avenue for fabricating synthetic protein hydrogels with integrated features.