Mg-Al-Ti layered double hydroxides (LDH), consisting of di-, tri- and tetra-valent cations with different Al3+/Ti4+ ratio, have been synthesized by co-precipitation which was demonstrated as efficient visible-light photocatalysts. The structure and chemical composition of the compound were characterized by PXRD, FT-IR, SAA, N2 adsorption-desorption isotherms, and DSC techniques. It is found that no hydrotalcites structure were formed for Ti4+/(Ti4++ Al3+)>0.5 and the substitution of Ti(IV) for Al(III) in the layer increases the thermal stability of the resulting LDH materials. The calcined sample containing titanium showed relatively high adsorption capacity for MB as compared to that without titanium. Results show that the pseudo-second-order kinetic model and the Langmuir were found to correlate the experimental data well. The photocatalytic activity was evaluated for the degradation of the methylene blue. The photocatalytic activity increased with the increase of the Al/Ti cationic ratio. 71% of the dye could be removed by the Mg/Al/Ti-LDH with the cationic ratio Al/Ti=0 : 1 and calcined at 500 ℃.