A series of TiO2/MgZnAl photocatalysts were successfully synthesized from ternary (Mg, Zn and Al) layered double hydroxides impregnated with 79% nanoparticles by the co-precipitation method at variable pH with different Zn2+/Mg2+ molar ratios. The composite photocatalysts were calcined at 500 degrees C resulting in the incorporation of oxide zinc, in the calcined MgZnAl LDH structure. Synergistic effect between ZnO and TiO2 lead to significant enhancement of TiO2/MgZnAl photocatalytic activity. Composite photocatalysts were characterized by ICP-MS, N-2 adsorption-desorption, XRD, SEM, EDS, IR and UV-vis DRS. Phenol in aqueous solution (50 mg/L) was used as a model compound for evaluation of UV-vis (filter cut-off for lambda>300 nm) photocatalytic activity. The most efficient photocatalyst composite was obtained at a 5% Zn2+/Mg2+ molar ratio, in the catalyst identified as TiO2/MgZnAl-5. This composite catalyst had high photocatalytic activity, completely destroying phenol and removing 80% of total organic carbon in solution after 360 min. The TiO2/MgZnAl-5 catalyst remained relatively stable, presenting a 15% decrease in phenol degradation efficiency after five consecutive photocatalytic cycles. (C) 2015 Elsevier B.V. All rights reserved.