Up to now, the use of TiO2 has been considered a promising advanced technology for organic pollutants removal from air or water, since it has high biological and chemical stability, high photoactivity, low toxicity, and low-cost production. However, there are issues to be addressed in enhancing TiO2 performance, and one of the current key issues is redesigning UV-active photocatalysts and making them active in the visible region of the electromagnetic spectrum. This way, solar light absorption will be insured, and thus, a more efficient photocatalyst could be obtained. For this reason, conjugated polymers and their derivatives are considered to act as photosensitizers, being able to shift the TiO2 activity from the UV to the visible region. Therefore, this study focuses on the synthesis of TiO2/conjugated polymer systems, which was accomplished by the deposition of poly-3,4-ethylene-dioxy-thiophene (PEDOT [-C6H4O2S-]n), a low-band semiconductor with an excellent stability due to its extending π-conjugated electron system, on titania nanoarchitecture. First of all, a TiO2 nanoarchitecture was synthesized by an ultrasound-assisted sol–gel method. Then, TiO2/PEDOT systems were obtained and characterized by using different techniques such as X-ray diffraction, Fourier Transform Infrared Spectroscopy, Scanning Electron Microscopy, UV–Vis diffuse reflectance, and N2 sorption measurements. The synthesized composites confirmed their mesoporosity and lower band gap values compared to bare titania, which clearly shows the ability to work as photocatalysts under visible-light activity. Further, we demonstrated that an organic pollutant, Congo Red dye, used as a model molecule could be photodegraded with the synthesized TiO2/PEDOT systems, with efficiencies of up to 95% in the case of TconvPEDOT under UV light and up to 99% for TconvPEDOT under visible-light irradiation, accomplishing in this way a successful synthesis of visible-light-activated titania photocatalyst.