Reflow-Resistant Self-Healing Microstructured Nanocomposite Conductors for Robust Bioelectronic Interfaces

The development of intrinsically self-healable polymeric adhesives has opened new opportunities for skin-interfaced bioelectronics; however, uncontrolled polymer flow and rapid chain relaxation often compromise structural integrity and long-term adhesion. Herein, we report a flow-controlled supramolecular nanocomposite adhesive with hierarchically self-assembled reinforcing nanostructures that simultaneously achieves softness, structural stability, and autonomous self-healing. By incorporating single-walled carbon nanotubes into a dynamic supramolecular polymer network, the nanocomposite regulates molecular mobility while promoting hierarchical nanostructure formation, enabling excellent resistance to reflow without sacrificing elasticity. The resulting material exhibits a low Young's modulus (~425 kPa), robust dimensional stability under pressure, water immersion, and mild heating for over 7 days, together with efficient self-healing capability. Furthermore, a double-layered cephalopod-inspired adhesive architecture programs interfacial adaptability and energy dissipation, providing reliable adhesion across wet, rough, and dynamically deforming surfaces. The stable adhesive interface enables continuous electrocardiogram and electromyogram monitoring as well as robotic control under swollen, aged, and healed conditions, demonstrating the potential of structure-engineered supramolecular nanocomposites for advanced wearable bioelectronics.