Design of functional hydrogels using smart polymer based on elastin-like polypeptides

In this work, we described an integrated experiment-modeling-application approach systematically based on genetically encoded elastin-like polypeptides (ELPs) for producing dynamic biomaterials with desired functions. Through the modification of methacrylate group, primitive lysine-rich ELPs acquired lower transition temperature and photo-crosslinking capabilities. [Display omitted] •Lysine-rich ELPs were synthesized using recombinant DNA technology.•Through modification of MA, ELPs acquired lower Tt and photo-crosslinking ability.•Molecular modeling and simulation were used to explore the conformation change.•ELP-MA can be engineered as light transmittance regulator and elastic adhesives. Elastin-like polypeptides (ELPs) are genetically encoded materials that enable the bottom-up design and manufacture of functional biomaterials. Here, we report the design and synthesis of a lysine-rich ELPs modified with methacrylate groups, giving rise to temperature-induced phase transition and photo-crosslinking capabilities. The degree of methacrylate functionalization could be varied by changing the reactant ratio of N-succinimidyl methacrylate (NHS-MA) to ELPs. The prediction of the structural transition with increasing temperature was validated using integrated experimental and simulation approaches. Combined with hydrogel fabrication strategy, methacrylated ELPs (ELP-MA) can be engineered into different physical forms like coacervates and hydrogels, which further function as light transmittance regulator and elastic adhesives. In addition, physical properties of the hydrogels such as mechanical strength, pore size, and swelling ratio could be controlled by the methacrylation degree and ELP-MA concentration. Subcutaneous implantation in mice showed that the resulting ELP-MA hydrogels exhibited a good biocompatibility. Our biological and chemical engineering approaches to creat functional materials of the ELP-MA will be useful to design various smart materials in the future.