Autonomous alignment and self-healing in multilayer soft electronics using dynamic polymers with immiscible backbones

Self-healing soft electronic and robotic devices can recover autonomously from some forms of external damage, analogous to human skin. While current self-healing devices employ a single type of dynamic polymer network for all functional layers to ensure strong interlayer adhesion, this approach requires the manual alignment of layers to ensure functional healing. Here, we use two dynamic polymers, which have immiscible backbones but identical dynamic bonds, to maintain interlayer adhesion while enabling autonomous realignment of functional components during healing. We show that these dynamic polymers exhibit a weakly interpenetrating and adhesive interface, whose width is tunable. Moreover, when multi-layer laminates of these polymers are misaligned after damage, these structures autonomously realign during healing to minimize interfacial area—a phenomena that is also observed in simulations. We demonstrate the broader utility of this strategy by fabricating composite devices with conductive, dielectric, and magnetic particles that functionally heal after damage, enabling thin film pressure sensors, magnetically assembled soft robots, and underwater circuit assembly.