We present a systematic review of nanostructured organic materials, including synthesis methods, functionalization, and applications. First, we report the chemical and physical procedures used for preparing the polymer/carbon nanotube composites described in the literature over the last decade. We compare the properties of different polymer-based prototypes of organic nanocomposites functionalized with carbon nanotubes. Theoretical and experimental vibrational investigations provide evidence of the molecular structure describing the interaction between both components, showing that the allowed amount of carbon nanotubes and their dispersion states differ across polymers. Moreover, the nature of the solvent used in the preparation has a significant impact on the dispersion process. The integration of these materials in photovoltaic applications is discussed, where the impact of nanoparticles is evidenced through the correlation between experimental analyses and theoretical approaches based on density functional theory. Alterations in optical properties, evaluated from the absorption and luminescence process, are coherent with the solar spectrum, and a good distribution of donor/acceptor interpenetration was observed. In all cases, it was demonstrated that the performance improvement is physically related to the charge transfer from the organic matrix to the nanoparticles.