True solutions of carbon nanotubes are notoriously difficult to obtain and generally are best thought of as stable (or otherwise) suspensions. Typically, surfactants are used to ‘solubilise' nanotubes and allow stable suspensions to be produced. This, however, leads to their subsequent behaviour being affected by the surfactant. Surfactant-less solubilised nanotubes are also important for understanding their interactions with nanoparticles as their surface is unaltered by adsorbed molecules. We present a method of formation of stable solutions of multiwall carbon nanotubes (MWNT) and how these solutions can be used in the growth of pseudo-monolayer thin films of MWNT, without surfactant, with thicknesses on the order of 10 nm (figure 1). Controlled amounts of gold nanoparticles and functionalised MWNT can be incorporated in these films. These films can be grown over several square cm and are sufficiently robust to be transferred to electrode arrays where their electrical properties may be probed and device architectures assembled through the use of directing electrical or magnetic fields. We demonstrate that in order to understand the measurable physical properties such as electrical conductivity and to correlate these to the underlying structure of a film, it is important to characterise the film sample at nano-, meso- and macroscales. Figure 1 is an illustration of the types of structures formed when nanoparticles and MWNT assemble in differing systems; (a) in the solution phase, leading to discrete assemblies and (b) when constrained in two dimensions at an interface. Further aggregation processes occur over time, namely (c) the production of larger 3D aggregates which will precipitate (d) upon reaching a critical size. 2D films will be formed from direct assembly of individual components but also by coalescence of small discrete assemblies, (e), but do not go on to form precipitates, (f).