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Hydrogel-based strain sensors inspired by nature have attracted tremendous attention for their promising applications in advanced wearable electronics. Nevertheless, achieving a skin-like stretchable conductive hydrogel with synergistic characteristics, such as ideal stretchability, excellent sensing performance and high self-healing efficiency, remains challenging. Herein, a highly stretchable, self-healing and electro-conductive hydrogel with a hierarchically triple-network structure was developed through a facile two-step preparation process. Firstly, 2, 2, 6, 6-tetrametylpiperidine-1-oxyl (TEMPO)-oxidized cellulose nanofibrils were homogeneously dispersed into polyacrylic acid hydrogel, with the presence of ferric ions as an ionic crosslinker to synthesize TEMPO-oxidized cellulose nanofibrils/polyacrylic acid hydrogel via a one-pot free radical polymerization. A polypyrrole conductive network was then incorporated into the synthetic hydrogel matrix as the third-level gel network by polymerizing pyrrole monomers. The hierarchical 3D network was mutually interlocked through hydrogen bonds, ionic coordination interactions and physical entanglements of polymer chains to achieve the target composite hydrogels with a homogeneous texture, enhanced mechanical stretchability (elongation at break of ~890%), high viscoelasticity (maximum storage modulus of ~27.1 kPa), intrinsic self-healing ability (electrical and mechanical healing efficiencies of ~99.4% and 98.3%) and ideal electro-conductibility (~3.9 S m−1). The strain sensor assembled by the hybrid hydrogel, with a desired gauge factor of ~7.3, exhibits a sensitive, fast and stable current response for monitoring small/large-scale human movements in real-time, demonstrating promising applications in damage-free wearable electronics.

Conductive and self-healing hydrogels are among the emerging materials that mimic the human skin and are important due to their probable prospects in soft robots and wearable electronics. However, the mechanical properties of the hydrogel matrix limit their applications. In this study, we developed a physicochemically dual cross-linked chemically modi ed-cellulose nano bers-carbon nanotubes/polyacrylic acid (TOCNF-CNTs/PAA) hydrogel. The TOCNFs acted both as a nano ller and dispersant to increase the mechanical strength of the PAA matrix and break the agglomerates of the CNTs. The nal self-healing and conductive TOCNF-CNTs/PAA-0.7 (mass ratio of CNTs to AA) hydrogel with a uniform texture exhibited highly intrinsic stretchability (breaking elongation to ca. 850%), enhanced tensile properties (ca. 59kPa), ideal conductivity (ca. 2.88S•m − 1 ) and pressure sensitivity. Besides, the composite hydrogels achieved up to approximately 98.36% and 99.99% self-healing e ciency for mechanical and electrical properties, respectively, without any external stimuli. Therefore, the as-designed multi-functional self-healing hydrogels, combined with stretching, sensitivity, and repeatability, possess the ability to monitor human activity and develop multifunctional, advanced, and commercial products such as wearable strain sensors, health monitors, and smart robots.