Titanosilicates are the most representative metallosilicates and have been widely used as redox and solid-acid catalysts in various reactions. This chapter reviews titanosilicates with different topologies, along with their synthesis methods, including hydrothermal synthesis, dry-gel conversion, direct synthesis in fluoride media, and post-synthesis. The research on titanosilicate synthesis is primarily focused on increasing the content of isomorphously substituted Ti in frameworks, manipulating the coordination and distribution of Ti species, and enhancing the accessibility of these Ti active sites to generate highly active catalysts.