A novel open-framework ecomaterial silicotitanate (Na4Ti4Si3O10) was synthesized by a combination of solgel and hydrothermal methods. The investigation on ion exchange properties shows that Na4Ti4Si3O10 exhibits high adsorption for cesium, i.e., Kd is as high as 60 000 mL/g in neutral solution. The crystal structure of Na4Ti4Si3O10 was characterized by X-ray diffraction (XRD), scanning electronic microscope (SEM), transmission electron microscope (TEM),Raman spectrum, differential thermal and thermogravimetric analysis (DTA/TGA), inductively coupled plasma (ICP),and X fluorescence analysis. The compound is tetragonal, P42, a = b = 0.781 10 nm, c = 1.196 45 nm, a =β = γ = 90°, Z= 4, and Ra = 0.041; Na4Ti4Si3O10 has a three dimensional framework consisting of Ti-O octahedral clusters and Si-O tetrahedra. The results show that Na4Ti4Si3O10 has good chemical stability, thermal stability, and high cesium ion exchange capacity in the whole pH range.