Cover Story: Translating molecular chirality into tunable optical responses is central to developing advanced chiroptical materials. This review explores N-carboxyanhydride (NCA)-derived polypeptides as programmable platforms linking molecular design, hierarchical chiral assembly, and optical function. NCA ring-opening polymerization enables control over stereochemistry, chain length, architecture, and functionality, directing secondary structures and higher-order organization. Through secondary structures such as α-helices and β-sheets, molecular chirality extends across multiple length scales into superhelices, nanotoroids, liquid-crystalline phases, and ordered bulk materials. These organized environments can transfer chirality to covalently attached or noncovalently incorporated chromophores, enabling induced circular dichroism and circularly polarized luminescence. Examples spanning emissive liquid crystals, aqueous nanotoroids, and phosphorescent aggregates illustrate how conformation and supramolecular packing regulate chiroptical responses. This review highlights design principles, challenges, and opportunities for translating these relationships into functional materials, with potential applications in chiral sensing, polarization-resolved bioimaging, and transient/biodegradable optical systems.

Wang, S.; Zhang, M.; Kim, M.; Wu, W.; Lin, Z. N-Carboxyanhydride-Derived Polypeptides as Programmable Platforms for Hierarchical Chiral Assembly and Chiroptical Materials. Materials and Interfaces 2026, 3 (3), 313–332. https://doi.org/10.53941/mi.2026.100021