Biomimetic and Gel‐Mediated Tissue Adhesive Structures for Skin Conformal and Multifunctional Bioelectronics

Epidermal electrodes are essential for wearable bioelectronics in health monitoring and rehabilitation. However, current options are limited: adhesives irritate skin, hydrogels dry out, ultrathin films cannot deliver high currents, and sharp microstructures concentrate current, risking burns. Achieving repeatable gel‐mediated adhesion with uniform current distribution on curved, moving skin remains a major challenge. In this study, we present biomimetic electrodes using carbon nanotube‐silicone elastomer (CNT‐elastomer) composites patterned with octopus‐inspired suction units and polyethylenimine (PEIE)‐induced microwrinkles. With an interfacing electrolyte gel, these electrodes achieve strong, repeatable skin adhesion of up to 77 ± 5 J m −2 in the normal direction and maintain performance over 100 reapplication cycles. Charge‐transfer resistance across the skin is reduced by 20‐fold, establishing low‐impedance interfaces. The electrodes record electrophysiological signals with clinical‐grade fidelity and deliver surface functional electrical stimulation with 50% higher efficiency in large muscle groups. Manufactured through facile fabrication methods of mold casting and leaving no skin residue, the electrodes exhibit skin‐matching mechanical compliance and efficient charge transfer, advancing comfortable and durable bioelectronic interfaces for rehabilitation, assistive neurotechnology, and next‐generation healthcare devices.