This research presents a generic fabrication method for tailoring polymer/carbon nanofillers composites with controlled architecture and composition. Two types of common carbon nanofillers, i.e. multiâwalled carbon nanotubes (MWNTs) and graphene nanosheets, are finely dispersed in an aqueous dispersion of polyacrylate followed by a microfiltration process. The second step allows preserving the high dispersion level of the nanofillers within the polymer matrix in the resulting solid films/layers. This study aims to investigate the structureâproperty relationship of the polyacrylate/nanofiller films, fabricated by the combination of latex technology and microfiltration. The polyacrylate/MWNTs system is studied over the entire MWNTs composition (0 to 100âwt%) and is shown to exhibit a structural transition; from a nanocomposite structure, in which the nanotubes are dispersed within a continuous polymer matrix, to a porous MWNTs macrostructure containing segregated polymer domains. This structural transition is corroborated with the filmsâspecific surface area values and the mechanical properties versus the MWNTs content. The percolation threshold of the studied polyacrylate/MWNTs systems is obtained at MWNTs content of ~0.04âwt%, an order of magnitude lower compared with cast films, fabricated by conventional latex technology. Polyacrylate/graphene nanosheet nanocomposites that are fabricated using the same method also demonstrate a structural transition from nanofiller/polymer composite material to graphene macrostructures. Copyright © 2014 John Wiley & Sons, Ltd.