Water pollution is one of the global threats severely affecting our planet and human health. Organic textile dyes are one of the common organic water pollutants that are presentient to degradation by traditional physical methods. Semiconductor-assisted photocatalysis is considered a green, efficient, and sustainable technology for wastewater treatment. To maximize the efficient utilization of solar radiation, it is of pivotal significance to explore novel organic molecules to be employed as efficient dye sensitizers for wide-bandgap semiconductors to extend their performance to the Visible-light region. Hence, in this work, we are proposing the design and synthesis of novel structures of QAD molecule as a dye photosensitizer with extended visible light absorptivity due to the extended π–π/n–π conjugations, to promote the performance of TiO₂ nanoparticles to the visible-light region and enhance the charge separation. The physicochemical characterizations confirmed the successful synthesis of QAD, TiO_2, and QAD/TiO₂ samples with the proposed structures. The anchoring of QAD molecules on the surface of TiO₂ caused a substantial improvement in the optical characteristics of TiO₂ as well as overcoming its common drawbacks by decreasing its bandgap energy to 2.6 eV, a remarkable reduction of PL intensity indicating reducing the e–h recombination and enhancing the charge separation, and creation of efficient visible light-harvesting antenna in the range of 400–600 nm. Besides, the QAD/TiO₂ sample achieved a 3-fold enhancement in the observed rate constant of the photodegradation of Rhodamine B dye compared to the bare TiO₂. The parameters affecting the photodegradation process were optimized and the sample displayed outstanding stability after 4 consecutive cycles. Finally, the effect of the scavengers was investigated and $${\mathrm{O}}_{2}^{\cdot -}$$O 2 · - was proposed to be the most reactive species and the mechanism of the enhancement was suggested based on the electron injection from the QAD’s HOMO level to the TiO₂’s CB. Finally, this work opens the door for various studies for the investigation of the proposed structures or similar structures in various photocatalytic/biomedical applications.