Leaf‐Inspired Cellulose Ionogels Under Spatial Confinement with Synergistically Enhanced Mechanical and Sensing Performance for Flexible Sensors

Abstract Flexible sensing materials have garnered significant attention due to their application value in fields such as wearable electronics and medical monitoring. However, achieving a balance between mechanical performance and sensing performance remains a major challenge. Inspired by the vein network structure of Arabidopsis thaliana leaves and their ability to transmit electrical signals under mechanical stimulation, N, N‐dimethylacrylamide (DMAA), acrylamide (AM), and 1‐ethyl‐3‐methylimidazolium ethyl sulfate (EMIES) are introduced into a cellulose network skeleton, successfully preparing the microphase‐separated conductive ionogel through copolymerization. The solubility differences of polymer segments in ionic liquids induce microphase separation, while the spatial confinement effect of the cellulose skeleton regulated the growth and distribution of the microphase structure. The obtained ionogel exhibits excellent tensile strength (2.37 MPa) and toughness (4.27 MJ m −3 ). Meanwhile, the cellulose network structure positively contributes to ion transport ( σ EP 3 C 5 = 0.72 mS cm −1 ). The flexible sensor based on the EMIES/P(DMAA‐AM)/cellulose ionogel features a rapid response time (125 ms), good cycling stability, and environmental adaptability, enabling real‐time monitoring of human joint movements and facilitating human‐computer interaction. This spatial confinement strategy achieves synergistic enhancement of the mechanical properties and conductivity of ionogels, providing innovative insights for the design and application of high‐performance flexible sensors.