Conductive Reflow-Resistant Self-Healing Nanocomposite-Structured Adhesives for Reliable and Versatile Bioelectronic Interfaces

Skin-like wearable bioelectronics should exhibit stable adhesion, benign detachment, stretchability, and self-healability to meet the demands of future user-interactive electronic skin applications. Despite recent rapid advances in self-healable adhesive electronic materials, inherent flowability and fast chain dynamics still lead to inferior performance compared to nonself-healable systems. Herein, we present an architecturally stable, repositionable, and biocompatible reflow-controlled double-layered cephalopod-inspired adhesive electrode capable of autonomous self-healing. The reflow-resistant composite material consists of single-walled carbon nanotubes and supramolecular polymers that can control flowability and induce hierarchically self-assembled reinforced nanostructures, resulting in soft (Young's modulus: ∼425 kPa) yet dimensionally stable systems under various conditions (underwater, pressure, and mild heat) over 7 days. The versatile bioelectronic adhesive interface programmed based on surface adaptability and energy distribution can induce robust adhesion in various (wet, rough, and dynamic) environments. Based on intimate adhesion with the skin, we demonstrate electrocardiogram/electromyogram signal acquisition and robot manipulation during dynamic motion under swollen, aged, and healed conditions.