Abstract:To address the longstanding challenge of simultaneously enhancing mechanical stability, low-temperature ionic conductivity, and interfacial reliability of hydrogel electrodes for triboelectric nanogenerators (TENGs), a poly(vinyl alcohol) (PVA)-polyethyleneimine (PEI)-phytic acid (PA)-montmorillonite (MMT) nanocomposite hydrogel based on multiple dynamic noncovalent interactions was developed. By synergistically introducing PEI, PA, and MMT nanosheets into a freeze-thaw PVA network, a hierarchical and dynamically crosslinked physical network was constructed, enabling the concurrent optimization of multiple functional properties. The resulting hydrogel exhibits excellent mechanical performance with a fracture stress of up to 0.69 MPa, high ionic conductivity (~2.5 S/m at room temperature), and stable flexibility and conductivity (~2.3 S/m) even at ?20 °C. In addition, the hydrogel demonstrates robust and universal adhesion to various substrates, along with an intrinsic self-healing capability. A TENG fabricated using this hydrogel as the electrode delivers stable electrical output and good cyclic durability. This work provides a viable design strategy for high-performance anti-freezing conductive hydrogels and expands their potential applications in flexible self-powered electronic devices.