EGaIn‐Activated Bioinspired Silk Micro/Nanofibril Eutectogels Breaking the Strength–Conductivity Trade‐Off for High‐Performance Wearable Bioelectronics

Eutectogels combining high mechanical and electrical performance hold great promise for next-generation wearable electronics. However, conventional polymerizable deep eutectic solvent (PDES)-based eutectogels suffer from an inherent strength-conductivity trade-off. Here, inspired by the multiscale architecture of the extracellular matrix, a bioinspired strategy is developed by integrating silk micro/nanofibrils (SMNF) as a reinforcing scaffold within a choline chloride/acrylic acid PDES. SMNF are generated in situ via deconstruction of silk fibers, while eutectic gallium-indium (EGaIn) microdroplets initiate polymerization without toxic initiators or high-energy UV irradiation, enabling one-step fabrication of SMNF-reinforced eutectogels (SMNF-Egel). The resulting SMNF-Egel combines dynamic hydrogen and coordination bonding with a robust micro/nanofibrous network, achieving a tensile strength of 1.25 MPa, toughness of 23.09 MJ m^-3, fracture strain of 2289%, and conductivity of 1.51 S m^-1, alongside skin-like modulus, self-healing, and environmental stability. These properties enable ultrasensitive strain sensing, Morse code communication, and stable bioelectrical signal monitoring. This work establishes a sustainable route to high-performance silk-based eutectogels and provides a versatile platform for advanced wearable sensors and bioelectronic interfaces.