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Synthetic peptides, designed from scratch, are valuable building blocks for the fabrication of artificial nanoscale architectures. In recent years, the designed peptides have been applied to intracellular applications such as protein labelling, controlling of protein activation and assembly, and as drug carriers, etc. This chapter summarizes some recent reports to highlight progress in the de novo design of coiled-coil peptides, small synthetic peptides, and β-sheet peptides used in living cells or in vivo.

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