Hydrogels with Hyperelasticity Engineered via Molecular Engineering of Dissipative Energy

Abstract Noticeable progress has been made in mechanically strong and tough of polymer gels, whereas this consistency between mechanical robustness and perfect elasticity remains a challenge. Here, a simple method is conducted for fabricating hyperelastic hydrogels based on the proposed molecular engineering of dissipative energy taking advantage of two distinct interactions with great difference of binding energy. This molecular engineering of dissipative energy refers to the complementarity at the molecular level between strong and weak interactions: the strong interaction provides the mechanical strength, the weak interaction eliminates the yielding and dense chain entanglements are further implanted, resulting in the perfect hyperelasticity. Such a complementarity in reformation time and binding energy of two interactions triggers a wide range of controllable window for regulating mechanical performances, filling the current gap in the design of hyperelasticity using only high‐order structures. The resultant hyperelastic hydrogels exhibit remarkable tensile strength and linear elastic deformation, but also outstanding swelling resistance, biocompatibility, hydrophilicity, and skin‐like elastic moduli. The work thus provides a promising concept for designing elastic and robust polymer gels and brings a new perspective in the combination of mutually incompatible mechanical properties, which will likely promote innovative applications in bioengineering and bioelectronics.