Molecular‐Scale Design of Cellulose‐Based Functional Materials for Flexible Electronic Devices

Abstract Structural design and self‐assembly at the molecular level provide feasible strategies for constructing materials with novel and unique properties. Cellulose is one of the most abundant bioresources and is renewable, biodegradable, biocompatible, and environmentally friendly. The formation of hydrogen‐bonding networks between the cellulose molecular chains on the one hand gives cellulose a rigid crystalline region and high mechanical strength and on the other hand it causes inconvenience to material design based on the molecular scale. The emergence of eco‐friendly solvents such as ionic liquids and alkali/urea solutions breaks the hydrogen bonds and allows the design of various cellulose‐based functional materials, such as membranes, gels, fibers, and nano/microspheres via structural optimization and molecular self‐assembly. Such functional materials have promising applications in flexible electronic devices, such as electrochemical energy storage devices, sensors, biomimetic electronic skins, and optoelectronic devices. In this review, green solvents for cellulose, the dissolution–recombination process, molecular self‐assembly strategies, advanced applications, and future development prospects for high‐performance cellulose‐based functional materials with unique structures are presented.