Tb-TNSs with high stability and regeneration behavior were prepared by one-pot method. Loaded TbxOy nanoparticles lead to obvious increase of the Ti3+ ions content. Loaded TbxOy results in the changes in the structure of the TNSs and red shift. Loaded TbxOy can effectively trap electrons to enhance the separation of charges. Tb-TNSs exhibit excellent synergistic photocatalytic activities for Cr(VI) and phenol.