Comb-like poly (beta-aspartate)s that adopt layered arrangements with well-defined phase transitions are revealed here. Outstanding thermochromic effects are displayed by these materials under polarized light, with a rapid, fully reversible color response that is highly sensitive to temperature (see Figure) and that can be adjusted by copolymerization. [GRAPHICS] Supramolecular Layered Structures of Comb-like Poly(beta-peptide)s Showing Thermochromic Properties.