Ultra‐Tough and Ultralow‐Hysteresis Liquid Crystalline Nanocomposite Stretchable Ionogels Constructed by Attapulgite Nanorods Assisted Mixed‐Ionic Liquids‐Induced Phase Separation

ABSTRACT Traditional stretchable ionogels suffer from the trade‐off between mechanical toughness and elastic recoverability, severely hindering their practical applications in durable and resilient flexible ionotronics. Here, an ultra‐tough and ultralow‐hysteresis liquid crystalline nanocomposite stretchable poly(vinyl alcohol) (PVA) ionogel is realized by using the mixed‐ionic liquids‐induced phase separation method with attapulgite nanorods as the junction points. The as‐prepared ionogels achieve ultrahigh toughness of 87.28 MJ/m 3 , extraordinary tensile strength of 13.58 MPa, high stretchability of 2320%, and ultralow‐hysteresis (5.9%‐8.7%), outperforming most reported stretchable ionogels. Importantly, the nanocomposite ionogels display strong birefringence with the integration of bright structural colors and mechano‐chromic performances. Moreover, the ionogel exhibits excellent ionic conductivity (up to 1.1 mS/cm), good reprocessability, and favorable healability. The application of these resilient ionogels as high‐performance flexible sensor for temperature/motion detecting and electrophysiological monitoring are further demonstrated, showing record high temperature sensitivity (up to 2237.8%/°C), high strain sensitivity (up to 6.69) over a wide range of detection from 1% to 700%, fast response time (83 ms), and excellent durability (3000 cycles). This ionogel demonstrates significant potential for application soft robotics, optical display electronics, and motion/temperature monitoring.