Graphene has shown to possess a host of extraordinary properties, such as high carrier mobility (15,000 cm2V–1s–1 [1]), high thermal conductivity (~5000 W/mK) [2], high mechanical properties (1 TPa Young’s modulus and 130 GPa tensile strength [3]) and non-permeability to standard gases [4], which promises to revolutionise many fields from optoelectronics to energy storage and generation, from sensors to transport (polymer composites for aerospace). And yet, the intrinsic properties of nanoparticles like graphene, are difficult to exploit due to major challenges in achieving precision, control and material design strategies that work for nanomaterials. In fact, we face a typical dilemma: the smaller the material’s dimensions, the more appealing its intrinsic physical properties, but also the more limited is our control over them. Herein we present a simple yet effective way, to produce nanocomposites with a well-defined micro and nanostructure based on a pastry making technique. The process, which we called “pressing and folding” (P&F), is an iterative top-down production technique whereby a filler and a binder are combined by successive pressing and folding steps. Not only is this process scalable, it also enables producing composites films with various compositions (up to 35 vol.%) and degree of organisation. In this work we study the processing of low density polyethylene, a widely used plastic, with graphene nano-platelets. We investigated the impact of the processing for various compositions on the final properties and established a theoretical model to predict the final properties based on the nano-filler dispersion level.