Elastic, Conductive, and Mechanically Strong Hydrogels from Dual-Cross-Linked Aramid Nanofiber Composites

Recent research on conductive hydrogels has revealed their potential for building advanced soft bioelectronic devices. Their mechanical flexibility, water content, and porosity approach those of biological tissues, providing a compliant interface between the human body and electronic hardware. Conductive hydrogels could be utilized in many soft tools such as neural electrodes, tactile interfaces, soft actuators, and other electroactive devices. However, most of the available conductive hydrogels exhibit weak mechanical properties, which hinders their application in durable biointegrated systems. Here, we report aramid nanofiber-based hydrogels providing a combination of high elasticity, strength, and electrical conductivity. Highly branched aramid nanofibers (ANFs) provide a robust three-dimensional (3D) framework resembling those in load-bearing soft tissues. When interlaced with poly(vinyl alcohol) (PVA) and cross-linked with both noncovalent and covalent interactions, the nanofiber composites exhibit a high water content of ∼76.4 wt %, strength of ∼7.5 MPa, ductility of ∼407%, and shape recovery of ∼99.5% under cyclic tensile stress of 0.3 MPa. Mobile ions impart a conductivity of ∼2 S/m to the hydrogels, enabling large-strain sensors with stable operation. In addition, the embedded silver nanoparticles afford broad-spectrum antimicrobial activities, which is favorable for medical devices. The versatility of aramid nanofiber-based composites suggests their further possibilities for functionalization and scalable fabrication toward sophisticated bioelectronic systems.