Soft bioelectronics that could be integrated with soft and curvilinear biological tissues/organs have attracted multidisciplinary research interest from material scientists, electronic engineers, and biomedical scientists. Because of their potential human health-related applications, soft bioelectronics require stringent demands for biocompatible components. Silk, as a kind of well-known ancient natural biopolymer, shows unique combined merits such as good biocompatibility, programmable biodegradability, processability into various material formats, and large-scale sustainable production. Such unique merits have made silk popular for intensive design and study in soft bioelectronics over the past decade. Due to the development of fabrication techniques in material processing and progress in research, silk has been engineered into a variety of advanced materials including silk fibers/textiles, nanofibers, films, hydrogels, and aerogels. Natural and regenerated silk materials can also be transformed into intrinsically nitrogen-doped and electrically conductive carbon materials, due to their unique molecular structure and high nitrogen content. The rich morphologies and varied processing options for silk materials can furnish transformed carbon materials with well-designed structures and properties. The favorable and unique material merits of silk materials and silk-derived carbon materials offer potential applications in soft electronics. Based on commercial silk fibers/textiles and the availability of re-engineered silk materials with versatile technological formats, functional soft electronics have been explored with silk as flexible biosupports/biomatrixes or active components. These soft systems include bioresorbable electronics, ultraconformal bioelectronics, transient electronics, epidermal electronics, textile electronics, conformal biosensors, flexible transistors, and resistive switching memory devices. Silk-derived carbon materials with rationally designed morphologies and structures have also been developed as active components for wearable sensors, electronic skins, and flexible energy devices, which provide novel concepts and opportunities for soft electronics. In this Account, we highlight the unique hierarchical and chemical structure of natural silk fibers, the fabrication strategies for processing silk into materials with versatile morphologies and into electrically conductive carbon materials, as well as recent progress in the development of silk-based advanced materials (silk materials and silk-derived carbon materials) for soft bioelectronics. The design and functionality of soft electronics developed with commercial silk fibers/textiles, re-engineered silk materials, and silk-derived carbon materials as biosubstrate/matrix and active components is introduced in detail. We further discuss future challenges and prospects for developing silk-based soft bioelectronics for wearable healthcare systems. By leveraging the unique advantages of silk-based advanced materials, the design and construction strategy for flexible electronics, as well as the potential of flexible electronics for conformable and intimate association with human tissues/organs, silk-based soft bioelectronics should have a significant impact on diverse healthcare fields.
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