Abstract
Self-healing hydrogels hold promise for smart sensors in bioengineering and intelligent systems, yet balancing self-healing ability with mechanical strength remains challenging. In this study, a self-healing hydrogel exhibiting superior stretchability was developed by embedding a combination of hydrogen bonding and dynamic metal coordination interactions, introduced by modified fenugreek galactomannan, ferric ions, and lignin silver nanoparticles, into a covalent polyacrylic acid (PAA) matrix. Synergistic covalent and multiple non-covalent interactions enabled the hydrogel with high self-healing ability and enhanced mechanical property. In particular, due to the introduction of multiple energy dissipation mechanisms, particularly migrative dynamic metal coordination interactions, the hydrogel exhibited ultra-high stretchability of up to 2000%. Furthermore, with the incorporation of lignin silver nanoparticles and ferric ions, the hydrogel demonstrated excellent strain sensitivity (gauge factor ≈ 3.94), with stable and repeatable resistance signals. Assembled into a flexible strain sensor, it effectively detected subtle human motions and organ vibrations, and even replaced conductive rubber in gaming controllers for real-time inputs. This study provides a versatile strategy for designing multifunctional hydrogels for advanced sensing applications.