Biomass and Transparent Supramolecular Elastomers for Green Electronics Enabled by the Controlled Growth and Self‐Assembly of Dynamic Polymer Networks

Determining the optimal method for preparing supramolecular materials remains a profound challenge. This process requires a combination of renewable raw materials to create supramolecular materials with multiple functions and properties, including simple fabrication, sustainability, a dynamic nature, good toughness, and transparency. In this work, a strategy is presented for toughening supramolecular networks based on solid‐phase chain extension. This toughening strategy is simple and environmentally friendly. In addition, a series of biobased elastomers are designed and prepared with adjustable performance characteristics. This strategy can significantly improve the transparency, tensile strength, and toughness of the synthesized elastomer. The synthesized biobased elastomers have great ductility, repairability, and recyclability, and they show good adhesion and dielectric properties. A biobased ionic skin is assembled from these biobased elastomers. Assembled ionic skin can sensitively detect external stimuli (such as stretching, bending, compression, or temperature changes) and monitor human movement. The conductive and dielectric layers of the biobased ionic skin are both obtained from renewable raw materials. This research provides novel molecular design approaches and material selection methods for promoting the development of green electronic devices and biobased elastomers. In this work, a strategy is presented for toughening supramolecular networks based on solid‐phase chain extension, and a green material system that combined hydrogen bonds and dynamic disulfide bonds is designed. The synthesized biobased elastomers have great ductility, repairability, and recyclability, and they show good adhesion and dielectric properties. Then a biobased ionic skin is assembled from these elastomers.