(a) Chemical structures of helical polypeptoids formed with chiral side groups and coiled polypeptoids formed with racemic side groups. The helical persistence length was a correlation distance along the helical contour, while the coiled persistence length was along the polymer chain contour, suggesting that helices made the polypeptoids segment more locally stiff in chain conformation while the chain remained overall flexible. Adapted with permission from ref. [18]; copyright © 2019 American Chemical Society. (b) Illustration of poly(n-butyl acrylate) (PnBA)-b-polypeptoids forming hexagonally packed cylinders, where helical polypeptoids block increased D-spacing due to unfavorable packing conditions due to chain stretching. Adapted with permission from ref. [15]; copyright © 2018 American Chemical Society. (c) Demonstration of polystyrene (PS)-b-polypeptoid self-assembled into different nanostructures and a helical interfacial segment shifted the self-assembly window towards a more significant polypeptoids volume fraction with narrower gyroids region. Adapted with permission from ref. [17]; copyright © 2021 American Chemical Society. (d) Representation of PnBA-b-polypeptoids self-assembled into lamellae structures with lower thermal stability against disordering, indicating unfavorable chain stretching in forming lamellae morphology. Adapted with permission from ref. [18]; copyright © 2019 American Chemical Society. (e) Schematic PS-b-polypeptoid diblock copolymer with non-compatibilized and compatibilized polypeptoid segments to form lamellae structures with widening intermixing regions. Adapted with permission from ref. [19]; copyright © 2020 American Chemical Society.