Despite there being a significant development in polymer composites for multiple applications over the past few decades, there are still many difficulties relating to the effective distribution of nanoparticles such as Graphene and other 2D materials in preparing structure and minimising aggregation. To overcome these obstacles a simple method for modulating the properties of the composites by controlling the organization of the fillers, using an ordered lattice of polymer particles as a template, is described. This technique can facilitate the self-assembly of nanomaterials while preserving their useful properties and allows well-defined interface between the polymer and the nanomaterial resulting in a honeycomb-like arrangement. The ideal case would be to obtain a segregated percolating network whereby low loadings of nanoparticles are added to obtain high performance systems and thus reduce the cost for possible industrial applications. The enhancement of the mechanical and electrical properties of the composites suggests the use of these materials for different applications such as transport applications, where the combination of high strength and lightweight is required. Moreover, to reinforce systems that are very delicate such as membranes or fibres or for possible applications in sensor technology, molecular electronics, supercapacitors, electrochromic devices and pressure sensitive adhesives materials. The physical properties of these composites can be tailored using different matrices such as natural rubber, or a bimodal particle system, to create materials with high density and low void fractions, and hence very low percolation threshold. Furthermore, the combination of excellent monolayer fraction and homogenous dispersion of the GO within the polymer dispersion leads to highly uniform films, with good distribution of the filler throughout, in a segregated network. A reduction in situ proceeds to improve the innate properties of the GO, but also to modify the polymer in close proximity through and exothermic process, thus providing a much improved interface between filler and matrix, improving both the electrical and mechanical properties. The advantage of this method to organize the graphene nanoparticles in a segregated pathway does not require the use of expensive equipment or materials, and it is a promising way to open up pathways to tunable electronic composite materials on a large scale
