Ultrasoft Yet Tough Multifunctional Organohydrogels Enabled by Molecular Chain Lubrication Strategy for Self‐Powered Wearable Electronics

ABSTRACT Flexible triboelectric nanogenerators (TENGs) underscore the promise of skin‑inspired hydrogels as intelligent materials for wearable electronics. However, overcoming the intrinsic trade‑off between stiffness and toughness while integrating multifunctionality into the hydrogels remains a great challenge. Here, we propose a multifunctional supramolecular organohydrogel (AQGL) via a molecular chain lubrication strategy, where glycerol (Gly)/water clusters act as dynamic lubricants to modulate polymer interactions and cross‑linking structure within the HAPAA/QCS/LiCl (AQL) gel network. This regulation endows the AQGL with remarkable mechanical characteristics, yielding an ultrahigh stretchability (5800%), ultralow Young's modulus (14.3 kPa), high toughness (11.77 MJ/m 3 ), and impressive fracture energy (75.96 kJ/m 2 ). Meanwhile, the AQGL further demonstrates multifunctionality including excellent optical transparency (∼95%), exceptional environmental durability against drying/freezing (−40°C), notable anti‐icing capability, distinguished antibacterial activity, high conductivity, and good self‐healing property. When employed as a TENG electrode, its intrinsic self‐adhesiveness ensures strong interfacial stability with triboelectric layer, enabling excellent electrical output and reliable performance in motion monitoring, handwriting recognition, and autonomous energy harvesting. This study provides a rational design strategy toward soft yet tough, and multifunctional organohydrogels, advancing the development of self‑powered epidermal electronics.