Abstract
AbstractPeptides and nucleic acids with programmable sequences are widely explored for the production of tunable, self‐assembling functional materials. Herein we demonstrate that the primary sequence of oligosaccharides can be designed to access materials with tunable shapes and properties. Synthetic cellulose‐based oligomers were assembled into 2D or 3D rod‐like crystallites. Sequence modifications within the oligosaccharide core influenced the molecular packing and led to the formation of square‐like assemblies based on the rare cellulose IVII allomorph. In contrast, modifications at the termini generated elongated aggregates with tunable surfaces, resulting in self‐healing supramolecular hydrogels.
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