Titanium pillared montmorillonite (Ti-MMT) was prepared by sol-gel method using sodium montmorillonite (Na-MMT) and tetrabutyl titanate as matrix materials. The Ti-MMT were characterized by XRD, FTIR and SEM. Then, the effects of different adsorption conditions on the adsorption of Ni2+ and Mn2+ on Ti-MMT were investigated, and the effect of pH on Zeta potential and adsorption was emphatically analyzed. The mechanism of Ti-MMT adsorption of Ni2+ and Mn2+ was investigated. The results show that Ti-MMT has a large interplanar spacing (d001=2.94 nm); pH has a great influence on adsorption, and the removal rate of Ni2+ and Mn2+ increases with the increase of initial pH. At pH=7, the dosage of Ti-MMT is 5 g/L, the initial mass concentration of Ni2+ is 50 mg/L, and the adsorption time is 120 min at 318 K, Ni2+ adsorption capacity can reach 9.46 mg/g, and the removal rate can reach 94.59%. At pH=7, the dosage of Ti-MMT is 9 g/L, the initial mass concentration of Mn2+ is 50 mg/L, and the adsorption time is 180 min at 318 K, Mn2+ adsorption capacity can reach 4.82 mg/g, and the removal rate can reach 86.73%. In addition, Ti-MMT adsorption of both ions is more consistent with Temkin isotherm adsorption, and the pseudo-second-order kinetics model. The adsorption process is controlled by liquid membrane diffusion and intra-particle diffusion, and ion exchange chemisorption is dominant. Thermodynamic analysis shows that the adsorption of Ni2+ by Ti-MMT belongs to the process of spontaneous endothermic entropy increase, while Mn2+ belongs to the non-spontaneous process of increasing endothermic entropy.