Mg-bearing silicate precursor gels have been prepared by mixing 0.74 mol/L sodium metasilicate and 1.48 mol/L magnesium nitrate solutions. Caustic soda solution of 1.0 mol/L concentration was introduced to regulate pH. The magnesium nitrate solution was added dropwise to the sodium silicate solution in equi-volume at various pH values. Raw and heat-treated gels were characterized by XRF, TG-DTA, XRD and FE-SEM. As a result, gel compositions were dependent on pH values of mixing solutions. The pH value yielding stoichiometric forsterite composition, MgO/SiO2 = 2 was reached at pH 9.3. In addition, this value was pH 8.4 for stoichiometric enstatite composition, MgO/SiO2 = 1. With decreasing pH from 9.3, the ratio became less than 2 and forsterite and enstatite precipitated by heating the gels. With increasing pH from 9.3, the ratio became more than 2 and forsterite and periclase precipitated by heating the gels. DTA curves showed a characteristic exothermic peak centered at 700–900∘C, indicating relatively low temperature formation of crystalline phases due to the presence of polycondensed frame works of silicates in the precursor gels.