High‐Strength, High‐Conductivity, and Crack‐Resistant Ionic Conductors with Aligned Cellulose Fibers

Abstract Ionogels as ionic conductors have attracted extensive attention due to their excellent ionic conductivity, good thermal and electrochemical stability, and favorable non‐volatility compared to conductive hydrogels. However, ionogels with excellent conductivity usually suffer from low strength and modulus. Herein, a facile yet effective strategy by compositing aligned cellulose fibers with ionogels is presented to achieve superior mechanical properties and high ionic conductivity. The triple hydrogen bond networks enable the ionic conductors to possess superhigh tensile strength (≈32.75 MPa) and Young's modulus (≈1354 MPa), as well as exhibit excellent crack‐resistant properties. Meanwhile, the ionic conductors with aligned cellulose fibers provide oriented hierarchical micro‐ and nanochannels for accelerating ion transport and thus can obtain a high ionic conductivity. Moreover, the ionic conductors exhibit high optical transparency (≈92%), good adhesion, and favorable flexibility. This work provides a straightforward and effective strategy for the development of high‐strength, high‐conductivity, and crack‐resistant ionic conductors.