Bioinspired nacre-like nanocomposite hydrogels via constrained self-assembly: Synergistic mechanical, thermal, and electrical properties

Developing conductive hydrogels capable of stable operation under mechanical deformation and temperature fluctuations represents a critical challenge in the fields of wearable and implantable electronics. Inspired by the “soft-hard-soft” layered heterogeneous architecture of natural nacre, we reports a nanocomposite hydrogel fabricated via a constrained self-assembly strategy. This strategy guides the spatiotemporal ordering of rigid nanofibers and a soft polymer network, successfully replicating the multi-level, nacre-like architecture. This distinct structure endows the material with synergistically enhanced multifunctionality, namely, exceptional tensile strength (0.6 MPa), superior toughness (32.81 MJ m⁻³), enhanced thermal conductivity (0.753 W·m⁻¹·K⁻¹), significant thermal stability (thermal decomposition temperature ~ 115.27 °C) and favorable electrical conductivity (12 S m⁻¹). As a proof of concept, based on the aforementioned outstanding performance, this hydrogel has been demonstrated to function as a strain sensor, effectively monitoring human joint movements such as those of the fingers, wrists, and elbow in real time. This work establishes a “bioinspired design–constrained assembly” paradigm for creating next-generation robust materials for flexible electronics.