Supramolecular‐Engineered Bamboo Lignin Polymer with Enhanced Mechanical and Electrical Properties for Flexible Electronics

A lignin‐derived ionogel is developed through a straightforward, one‐step solvent‐free process. By leveraging arginine‐grafted lignin‐terminated polythioctic acid and incorporating imine and hydroxyl groups into the supramolecular framework. Its dynamic disulfide/hydrogen‐bond dual networks enable balanced stretchability‐reversibility while delivering adhesion, conductivity, and self‐healing. This molecularly engineered system establishes a sustainable platform for next‐generation flexible sensors in wearables, e‐skin, and soft robotics. Abstract Ionogels have emerged as a groundbreaking category of materials for flexible electronics, yet the challenge of integrating high mechanical stretchability, rapid electrical response, and reliable self‐repair in bio‐based ionogels persists. Here, a lignin‐derived ionogel is presented, designated P(LA‐TA)‐gel, through a straightforward, one‐step solvent‐free process. By leveraging arginine‐grafted lignin‐terminated polythioctic acid and incorporating imine and hydroxyl groups into the supramolecular framework, the P(LA‐TA)‐gel with both dynamic disulfide bonds and supramolecular hydrogen bonds achieves effective energy dissipation channels. This configuration adeptly balances mechanical stretchability—exhibiting a strain of 1233%—with dynamic reversibility, evidenced by an adhesion strength of 335.5 kPa. Notably, the P(LA‐TA)‐gel showcases rapid response characteristics, achieving a response time of 0.1 s, along with high ionic conductivity of 17.36 mS cm−1 and robust self‐healing capabilities exceeding 90%. When utilized in flexible sensors, this ionogel demonstrates a wide response range and high sensitivity. This study establishes a sustainable platform for the development of next‐generation flexible sensors and highlights significant potential applications across wearable electronics, electronic skin technology, and soft robotics. A lignin-derived ionogel is developed through a straightforward, one-step solvent-free process. By leveraging arginine-grafted lignin-terminated polythioctic acid and incorporating imine and hydroxyl groups into the supramolecular framework. Its dynamic disulfide/hydrogen-bond dual networks enable balanced stretchability-reversibility while delivering adhesion, conductivity, and self-healing. This molecularly engineered system establishes a sustainable platform for next-generation flexible sensors in wearables, e-skin, and soft robotics. Abstract Ionogels have emerged as a groundbreaking category of materials for flexible electronics, yet the challenge of integrating high mechanical stretchability, rapid electrical response, and reliable self-repair in bio-based ionogels persists. Here, a lignin-derived ionogel is presented, designated P(LA-TA)-gel, through a straightforward, one-step solvent-free process. By leveraging arginine-grafted lignin-terminated polythioctic acid and incorporating imine and hydroxyl groups into the supramolecular framework, the P(LA-TA)-gel with both dynamic disulfide bonds and supramolecular hydrogen bonds achieves effective energy dissipation channels. This configuration adeptly balances mechanical stretchability—exhibiting a strain of 1233%—with dynamic reversibility, evidenced by an adhesion strength of 335.5 kPa. Notably, the P(LA-TA)-gel showcases rapid response characteristics, achieving a response time of 0.1 s, along with high ionic conductivity of 17.36 mS cm −1 and robust self-healing capabilities exceeding 90%. When utilized in flexible sensors, this ionogel demonstrates a wide response range and high sensitivity. This study establishes a sustainable platform for the development of next-generation flexible sensors and highlights significant potential applications across wearable electronics, electronic skin technology, and soft robotics. Advanced Science, Volume 12, Issue 43, November 20, 2025.