Abstract: Stretchable and compliant interference coatings for flexible optics and optoelectronic devices comprise polymeric optical thin films prepared by initiated chemical vapor deposition (iCVD) forming uniform, multilayered thin film coatings on temperature sensitive substrates at low temperature with precise thickness control. A model two-layer coating of poly(1H,1H,6H,6H-perfluorohexyl diacrylate) (pPFHDA) with a refractive index at 633 nm of n633=1.426 deposited onto poly(4-vinylpyridine) (p4VP, n633˜1.587) gives broadband performance over the visible wavelength range (400 nm to 750 nm) of a transparent, flexible thermoplastic polyurethane (TPU) substrate (n633˜1.51), reducing the front-surface reflectance from ˜4% to ˜2%, with superior mechanical compliance over conventional inorganic coatings (MgF2, SiO2, and Al2O3). Like interference coatings or three or more layers can be fabricated, where the materials and thicknesses of the layers can differ.