Bioinspired Structural Design Enables Synergistic Toughness and Conductivity in Hydrogels for Advanced Wearable...

Conductive hydrogels are revolutionizing the fields of wearable sensors, implantable bioelectronics, and soft robotics. However, achieving both mechanical robustness and high conductivity within a single system remains challenging. Here, inspired by the cooperative vascular-neural networks in biological tissues, we develop a nanofiber-reinforced conductive hydrogel composed of poly(vinyl alcohol) (PVA), aramid nanofibers (ANFs), and in situ polymerized PEDOT:PSS. Through solvent- and thermally induced structural reorganization, the hydrogel evolves into a bi-continuous architecture in which the mechanical and conductive networks are intimately coupled. The tough, ANF-reinforced porous PVA mimics the vascular system, providing mechanical support and maintaining toughness, while the poly(3,4-ethylenedioxythiophene) (PEDOT) network resembles neural pathways, enabling efficient electron transport. This structural evolution enables a rare synergy of high tensile strength (10.72 MPa) and ultrahigh conductivity (452.75 S m^-1) with excellent biocompatibility. The hydrogel maintains stable conduction under impact and complex deformation, supporting multimodal sensing from large-amplitude joint motion to low-amplitude electrophysiological signals: electrocardiographic and electromyographic. When integrated with a convolutional neural network, it achieves 99.54% accuracy in recognizing five complex hand gestures. This bioinspired strategy paves the way for developing robust and conductive hydrogels toward next-generation intelligent wearable electronics.