Materials and methods for forming self-assembled peptoid structures that are extremely stable, crystalline, free-standing and self-repairing are described. Based on the peptoid design, peptoid membranes in a 2D arrangement was able toroll into single-walled nanotubes with tunable sizes, diameters, thicknesses and stiffnesses as well as tailorable functions result. Crystalline nanomaterials made through this facile solution crystallization and anisotropic formation process are highly tailorable and exhibit a number of properties advantageous for applications such as water decontamination, cellular adhesion, imaging, surface coating, biosensing, energy conversion, biocatalysis or other applications.