Nanocomposite materials composed of a PTFE copolymer core and an acrylic copolymer shell have been prepared by seeded emulsion polymerization. The effect of seed particle number and shell polymer composition on secondary particle nucleation and film formation ability of the dispersions has been studied. While TEM reveals a core‐shell structure present in the particles, AFM investigation of the film shows a nearly uniform dispersion of the fluorinated seed particles in a matrix formed by the shell polymer. Rheological measurements show composite behavior of the core‐shell latex films, especially at elevated temperatures, and an increase in viscosity and storage modulus when compared with the properties of the pure acrylic component. These composites exhibit a solid‐like behavior at lower frequencies (in the rubbery zone) indicating the formation of a network‐like structure which acts as a reinforcement for the acrylic matrix. The process takes place faster at higher temperatures, probably due to the increased mobility of the cores and a corresponding improvement of the mechanical properties is observed. The fluoropolymer‐PBMA nanocomposite films also show opalescent crystal like behavior due to the existence of a refractive index gradient.