Titanosilicate molecular sieve (TS-1) is an important commercial catalyst for green production of oxyfunctionalized chemicals such as alcohols, ketones, epoxides, and oximes. Active TS-1 can normally be achieved in the synthetic media strictly free of alkali metal cations (e.g., Na+ and K+). This condition severely raises the purity demands of starting reagents, which greatly increases the production cost. Herein, we developed a method to achieve highly active titanosilicates in the presence of high-concentration alkali metal cations using anionic polymer-based quasi-neutral media. This synthetic route could effectively inhibit the adverse influence of alkali metal cations on the incorporation of active titanium(IV) sites into the framework of titanosilicate, directly affording the maximal framework titanium content (2.0 wt.%) with almost 100% yield. This development shows a great commercial potential and opens the possibility of preparing silica-based molecular sieves/zeolites in non-fluoride neutral media.