This study synthesized and characterized composites of graphene oxide and TiO2 (GO-TiO2). GO-TiO2 thin films were deposited using the Doctor Blade technique. Subsequently, the thin films were sensitized with a natural dye extracted from a Colombian source (Bactris guineensis). Thermogravimetric analysis, X-ray diffraction, Raman spectroscopy, scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and diffuse reflectance measurements were used for physicochemical characterization. All the samples were polycrystalline in nature, and the diffraction signals corresponded to the TiO2 anatase crystalline phase. Raman spectroscopy and FT-IR verified the synthesis of composite thin films, and the SEM analysis confirmed the TiO2 films morphological modification after the process of GO incorporation and sensitization. XPS results suggested a possibility of appearance of Titanium (III) through the formation of oxygen vacancies (Ov). Furthermore, the optical results indicated that the presence of the natural sensitizer and GO improved the optical properties of TiO2 in the visible range. Finally, the photocatalytic degradation of Methylene Blue (MB) was studied under visible irradiation in aqueous solution, and pseudo-first order model was used to obtain kinetic information about photocatalytic degradation. These results indicated that the presence of GO has an important synergistic effect in conjunction with the natural sensitizer, reaching a photocatalytic yield of 33%.