Conductive films comprising conducting polymers and carbon nanomaterials have gained a lot of interest for applications in several fields, including transparent electrodes, supercapacitors, light-emitting diodes (LEDs), polymer solar cells (PSCs), and so forth. One of the main motivations is the replacement of costly oxides and degradable materials, like indium tin oxide (ITO). On the other hand, graphene oxide (GO) has emerged as an ideal filler to reinforce polymeric matrices owing to its large specific surface area, transparency, flexibility, and very high mechanical strength. Nonetheless, functionalization is required to improve its solubility in common solvents and expand its practical uses. In this work, the potential of polymer nanocomposites based on hexamethylene diisocyanate (HDI)-functionalized GO (HDI-GO)/ poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)(PEDOT:PSS) for use as active layers (ALs) or interfacial layers (IFLs) in PSCs has been assessed. Conventional deposition techniques applied to thin films were tested for the developed nanocomposites. Deposition methods included drop and spin casting, where different type of substrates, as clean glass and glass/ITO were tested. The results of deposition essays were analyzed by atomic force microscopy (AFM) and UV-vis spectra. In addition, thermal evaporation was tried with the aim to obtain homogeneous layers. The layers obtained by drop casting showed poor film quality, with large aggregates. On the other hand, spin coating lead to layers not fully wetting the substrate. New synthesis procedures for the nanocomposites and/or alternative treatments of substrate surface will be investigated in the future to optimize their composition and properties (ie. transparency) and improve their suitability for use in PSCs.