Strain-Induced Phase Separation and Mechanomodulation of Ionic Conduction in Anisotropic Nanocomposite Ionogels

Ionogels have great potential for the development of tissue-like, soft, and stretchable ionotronics. However, conventional isotropic ionogels suffer from poor mechanical properties, low efficient force transmission, and tardy mechanoelectric response, hindering their practical utility. Here, we propose a simple one-step method to fabricate bioinspired anisotropic nanocomposite ionogels based on a combination of strain-induced phase separation and mechanomodulation of ionic conduction in the presence of attapulgite nanorods. These ionogels show high stretchability (747.1% strain), tensile strength (6.42 MPa), Young’s modulus (83.49 MPa), and toughness (18.08 MJ/m³). Importantly, the liquid crystalline domain alignment-induced microphase separation and ionic conductivity enhancement during stretching endow these ionogels with an unusual mechanoelectric response and dual-programmable shape-memory properties. Moreover, the anisotropic structure, good elasticity, and unique resistance–strain responsiveness give the ionogel-based strain sensors high sensitivity, rapid response time, excellent fatigue resistance, and unique waveform-discernible strain sensing, which can be applied to real-time monitoring of human motions. The findings offer a promising way to develop bioinspired anisotropic ionogels to modulate the microstructure and properties for practical applications in advanced ionotronics.