We demonstrated two complementary size-dependent structural coloring mechanisms, interference and scattering, in indefinitely long core-shell nanowire arrays. The unusual nanostructures are comprised of an amorphous semiconducting core and a polymer shell layer with disparate refractive indices but with similar thermomechanical properties. Core-shell nanowires are mass produced from a macroscopic semiconductor rod by using a new top-to-bottom fabrication approach based on thermal size reduction. Nanostructures with diameters from 30 to 200 nm result in coloration that spans the whole visible spectrum via resonant Mie scattering. Nanoshell coloration based on thin film interference is proposed as a structural coloration mechanism which becomes dominant for nanowires having 700-1200 nm diameter. Controlled color generation in any part of visible and infrared spectral regions can be achieved by the simple scaling down procedure. Spectral color generation in mass-produced uniform core-shell nanowire arrays paves the way for applications such as spectral authentication at nanoscale, light-scattering ingredients in paints and cosmetics, large-area devices, and infrared shielding. © 2011 American Chemical Society.