Highly stretchable dynamic hydrogels for soft multilayer electronics

Recent progress in the development of synthetic polymer networks has enabled the next generation of hydrogel-based machines and devices. The ability to mimic the mechanical and electrical properties of human tissue gives great potential toward the fields of bioelectronics and soft robotics. However, fabricating hydrogel devices that display high ionic conductivity while maintaining high stretchability and softness remains unmet. Here, we synthesize supramolecular poly(ionic) networks, which display high stretchability (>1500%), compressibility (>90%), and rapid self-recovery (<30 s), while achieving ionic conductivities of up to 0.1 S cm ^-1. Dynamic cross-links give rise to inter-layer adhesion and a stable interface is formed on account of ultrahigh binding affinities (>10¹³ M^-2). Superior adherence between layers enabled the fabrication of an intrinsically stretchable hydrogel power source, paving the way for the next generation of multi-layer tissue mimetic devices.