Green Solvent Systems for Cellulose Dissolution and Regeneration: Hydrogen‐Bond Engineering Toward Sustainable Functional Materials

Cellulose, the most abundant natural biopolymer, offers a sustainable alternative to petroleum-based products. However, its intrinsic and robust hydrogen-bonding network prevents thermal processing, severely hindering its practical use. Green solvent systems capable of disrupting this network under mild conditions without significant degradation have emerged as a transformative platform. This review provides a comprehensive analysis of cellulose dissolution, from its hierarchical supramolecular structure and swelling mechanisms to recent advances in green solvents, including ionic liquids and deep eutectic solvents. We highlight how solvation chemistry directly influences subsequent regeneration strategies (specifically solvent-induced phase transitions and thermally driven assembly), enabling precise control over hydrogen-bond reconstruction and molecular chain orientation. By bridging dissolution mechanisms with advanced manufacturing, this review elucidates design principles for creating high-performance cellulosic materials. We conclude with a forward-looking perspective on integrating artificial intelligence for solvent screening, scaling up sustainable processes, and realizing the full potential of cellulose-based smart materials in flexible electronics, biomedicine, and beyond.