Dynamic control of internarticle coupling within a single material comprising gold nanoparticles and poly(N-isopropylacrylamide) has been developed. Core/shell particles with defined shell thicknesses are the building blocks for preparing films of sufficiently high gold nanoparticle density necessary for achieving reversible switching of several optical properties simultaneously: color, transparency, and metallic luster. The polymer-shell architecture has a strong effect on particle and film stability.