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Peptide-based supramolecular self-assembly has been demonstrated to be a flexible approach for the fabrication of programmable de novo nanodrugs by employing synergistic or reciprocal intermolecular non-covalent interactions. This class of nanomaterials holds significant promise for clinical translation, especially as cancer theranostics. In this review, we describe the concept of cancer theranostic drug assembly by employing non-covalent interactions. That is, molecular drugs are formulated into nanoscale and even microscale architectures by peptide-modulated self-assembly. A series of peptide-based supramolecular assembly drugs are discussed, with an emphasis on the relation between structural feature and theranostic performance. Molecular design, manipulation of non-covalent interactions, and elucidation of structure-function relationships not only facilitate the implementation of supramolecular self-assembly principles in drug development, but also provide a new means for advancing anticancer nanostructured drugs toward clinical application.

Peptide-based supramolecular assembly drugs toward cancer theranostics