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High performance metakaolinite based cementitious materials were prepared with metakaolinite as main component, and the different modules of Na and Na-K silicate solutions as diagenetic agent. The results show that the mechanical properties are affected by different silicate solutions, compressive strengths of pastes hydrated for 3 d and 28 d with Na-K silicate solution (The modulus is 1) are about 43.68 and 78.52 MPa respectively. By analyzing the mechanical properties of Metakaolinite based cementitious materials, the diagenetic effect of lower module is better than higher module, and Na-K silicate solution is better than Na silicate solution. The structure of the Na and Na-K silicate solutions is studied with IR and 29Si NMR, the reason of the lower module and Na-K silicate solution improving the mechanical properties is that the low module silicate solution has lower polymeric degree of silicon dioxide, and the higher polymeric degree of silicon oxide tetrahedron(Q4) in Na-K silicate solution is less than Na silicate solution.