Calcium silicate hydrate (C-S-H) and magnesium silicate hydrate (M-S-H) have been described as two separate phases. This work investigates their stability domains and the possible uptake of small amounts of magnesium by C-S-H or, reversely, the uptake of small amounts of calcium by M-S-H. The phases, synthesized by co-precipitation, are characterized using a large panel of techniques (thermogravimetry analysis, X-ray diffraction, X-ray pair distribution function analysis, 29 Si MAS-NMR spectroscopy, 17 measurement of zeta potential and cation exchange capacity) while the compositions of the solutions at 18 equilibrium are determined by ion chromatography and pH measurements. Syntheses of C-S-H samples 19 in the presence of magnesium ((Ca+Mg)/Si = 0.8 and Mg/Si = 0.05 or 0.10) yield two separate phases: 20