This chapter discusses efforts along those lines and achievements in the formation of foldamer-based nanostructures in the aqueous environment. Helical foldamers are good candidates to build such artificial helix bundles. Mainly two approaches have been reported in the literature: a “top-down” approach, in which a natural peptide sequence known to form coiled coil structures is used as a starting scaffold to construct a nonnatural hybrid foldamer/peptide sequence that self-associates into bundles, or a “bottom-up” approach, in which the self-assembly is based on de novo designed amphiphilic foldamer helices with segregation of hydrophilic and lipophilic side chains. Several foldamer backbones were shown to render accessible elongated supramolecular nanostructures such as fibers, filament, and tubes akin to those formed by proteins and peptides. The chapter suggests the enticing opportunities for the creation of metal-coordinated nanostructures using appropriate oligomer sequences as foldable strands.