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This chapter highlights recent developments in enzyme-responsive gels. The focus is on peptide-based small-molecule hydrogels, for biomedical applications. The use of enzymes in this context provides a powerful methodology for controlled assembly, taking advantage of both biological selectivity and catalytic amplification. The building blocks for self-assembly and basic design rules for small molecule peptide gelators are discussed first. This is followed by a discussion of key features of biocatalytic self-assembly of hydrogels, focusing on control of nanoscale organization and consequent function. Finally, the potential applications of the enzyme-responsive hydrogels as biomaterials are discussed in the areas of cell culture, drug delivery, biosensing, and control of cell fate.

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