Poly(N-substituted glycine) "peptoids" have conventionally been exploited for drug discovery and therapeutics due to their structural similarity to peptides, protease resistance, and relative ease of synthesis. This mini-review highlights recent reports of peptoid self-assembled nanostructures and macromolecular interfaces relevant to biomaterials science. The results illustrate how the versatility of peptoid design and synthesis could be exploited to generate multifunctional, modular and precisely tunable biointerfaces and biomaterials.