In this work, heterostructured catalyst Al₂TiO₅/TiO₂ (ATO/Ti) was synthesized by a two-step method: low-temperature sol-gel process along with hydrothermal treatment in a neutral medium. Characteristics of the fabricated catalyst were analyzed by various techniques including X-ray diffraction, Fourier transform infrared spectroscopy, Brunauer-Emmett-Teller adsorption, UV-Vis diffuse reflectance spectroscopy, energy-dispersive X-ray spectroscopy, field emission scanning electron microscopy, transmission electron microscopy, Raman spectroscopy, and the point of zero charges. The content of ATO in ATO/Ti catalysts strongly affected the photocatalytic degradation of cinnamic acid (CA). The 33% ATO contained 33ATO/Ti catalyst exhibited the highest activity for the removal of CA. Compared with the bare TiO₂ synthesized in water (TiO₂(w)) as well as Al₂TiO₅ (ATO), the hybrid 33ATO/Ti catalyst exhibited enhanced photocatalytic activity in the CA degradation under ultraviolet light. The enhancement in the catalytic activity of ATO/Ti could be related to the increase of the specific surface area and the reduction of bandgap energy obtained from the hybridization of TiO₂(w)and ATO. The factors as the catalyst dosage (C_cat), the airflow rate (Q_air), and the solution initial pH (pH) affected the CA removal efficiency were studied on 33ATO/Ti catalyst. The optimum condition for photodegradation efficiency of CA was found to be at C_cat = 0.75 gL^-1, Q_air = 0.3 Lmin^-1, and pH = 3.8. The highest 60-minute removal efficiency of CA reached 77.1% on 33ATO/Ti, while the CA conversion was 67.1% on TiO₂(w) and 30.4% on ATO. The recyclability of the 33ATO/Ti was also measured at the optimal parameters. A significant decrease in the CA conversion of 35% after 6 continuous cycles.