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Cellulose, as the most abundant sustainable resource on earth, can be chemically transformed into a variety of biodegradable materials, which have been proposed as the ideal substitutes for plastic products. The first challenge for the fabrication of cellulose-based functional materials is the successful dissolution of cellulose by solvents. However, most existing cellulose solvents have environmental, economic, and other drawbacks that limit their further industrial applications. Research on developing novel solvent systems with “greener” and “cheaper” properties is needed to meet the challenges.