Ionic conductive gels are widely sought after for applications that require reliable ionic conduction and mechanical performance under extreme conditions, which remains a grand challenge. To address this limitation, we deliberately control water-induced hydration interactions within ionic liquid (IL)-based conductive gels (ionogels) to achieve all-round performance. Specifically, the competitive interactions between IL, water and cellulose nanofibrils (CNF) are balanced to preserve the nanoscale morphology of CNF while avoiding its dissolution. As a result, we synergistically enhance both mechanical performance and ionic conductivity of the resultant ionogel. For instance, an untrastretchable ionogel (up to 10250 412% stretchability) with both high toughness (21.8 0.9 MJ/m3) and ionic conductivity (0.70 0.06 S/m) is achieved. Furthermore, multimodal sensing functions (strain, compression, temperature, and humidity) are realized by assembling the ionogel as a skin-like membrane. Due to the low volatility of IL and its strong interaction with water, the ionogel maintains an excellent performance at either ultra-low temperature (-45 oC), high temperature (75 oC) or low humidity environment (RH &lt; 15%), demonstrating superb anti-freezing and anti-drying performance. Overall, we introduce a simple yet versatile strategy that leads to environmentally resilient ionogels to meet the requirements of next-generation electroactive devices.

Ultrastretchable ionogel with extreme environmental resilience through controlled hydration interactions

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