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Capturing the interfacial dynamics that drive the mechanical and biological properties of natural carbohydrate-based nanomaterials will require synergistic advances in 3D nanolithography, surface characterization, and organic and macromolecular chemistry at interfaces. The challenge, and the reason why this topic merits a Faraday Discussion, is that many of the researchers working in this area come from disparate fields that rarely if ever communicate, including physical chemistry, surface chemistry, mechanical engineering, biology, and material science.