LAUSR

Conductive hydrogels are promising interface materials utilized in bioelectronics for human–machine interactions. However, the low‐temperature induced freezing problem and water evaporation‐induced structural failures have significantly hindered their practical applications. To address these problems, herein, an elaborately designed nanocomposite organohydrogel is fabricated by introducing highly conductive MXene nanosheets into a tannic acid‐decorated cellulose nanofibrils/polyacrylamide hybrid gel network infiltrated with glycerol (Gly)/water binary solvent. Owing to the introduction of Gly, the as‐prepared organohydrogel demonstrates an outstanding flexibility and electrical conductivity under a wide temperature spectrum (from −36 to 60 °C), and exhibits long‐term stability in an open environment (>7 days). Additionally, the dynamic catechol‐borate ester bonds, along with the readily formed hydrogen bonds between the water and Gly molecules, further endow the organohydrogel with excellent stretchability (≈1500% strain), high tissue adhesiveness, and self‐healing properties. The favorable environmental stability and broad working strain range (≈500% strain); together with high sensitivity (gauge factor of 8.21) make this organohydrogel a promising candidate for both large and subtle motion monitoring.