Tl and As contamination in agricultural soils poses a significant threat to human health due to the exchangeable fraction readily assimilated by crops. In the present study, a batch experiment was set up with As and Tl contaminated soil in combination with two amendments (Fe-Mn binary oxides and Titanate nanomaterials), to evaluate the effects of the treatment on the mobility and bioavailability of Tl and As. The results of toxicity characteristic leaching procedure (TCLP) indicated that the Fe-Mn binary oxides exhibited the highest stabilization level for the exchangeable fraction of Tl and As (Tl=49.61% and As=53.01%). Fourier transformed infrared (FTIR) and X-ray photoelectron spectroscopy (XPS) spectra of Fe–Mn binary oxides suggested that it combined the oxidation property of manganese dioxide and the high adsorption features to As(V) of iron oxides, surface complexation, oxidation and precipitation were the main mechanisms for the stabilization of Tl, as for As, the main mechanisms were complexation and oxidation. After 7 days treatment of TNMs, more than 90% of exchangeable Tl was stabilized at TNMs dose of 3% (by dry weight), but it had no effect on As. Excellent Tl stabilization mainly depended on complexation of –ONa functional groups in the interlayers and Ti–OH on the surfaces of TNMs as well as ion exchange with Na⁺/H⁺. This study provides alternative potential in situ remediation strateies for both Tl and As stabilization in contaminated soils.