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Self-assembled hydrogels with extremely high water content (up to 99.5%) and highly tunable mechanical properties were prepared from renewable cellulose derivatives. These hydrogels are easily processed and the simplicity of their preparation, their availability from inexpensive renewable resources, and the tunability of their mechanical properties are distinguishing for important biomedical applications. The protein release characteristics were investigated to determine the effect of both the protein molecular weight and polymer loadings of the hydrogels on the protein release rate. Extremely sustained release of bovine serum albumin is observed over the course of 160 days from supramolecular hydrogels containing only 1.5 wt% polymeric constituents. This sustained release far surpasses the current state of the art for protein release from a hydrogel, highlighting these materials as important potential …