A crystalline substance which appears in steam-cured Portland cement mortar has been shown to be a calcium hydrosilicate and has been prepared by hydrothermal synthesis from mixtures of silica sand with lime, dicalcium silicate and tricalcium silicate, silica gel and lime (after preliminary steam treatment and ignition) and by the action of saturated lime water on quartz crystals or fused silica plates. The crystals appear not to be acted on by solutions of sodium sulphate, calcium sulphate or alkali hydroxides, but they are slowly decomposed by solutions of magnesium sulphate and alkali carbonates and rapidly by dilute acids and ammonium salts. The crystals were obtained free from amorphous matter by growing them on quartz or silica plates in saturated lime water. When the compound was prepared in this way, the lime-silica-water ratio was found to be 2:1:1, the formula being therefore 2CaO∙SiO2∙H2O or H2Ca2SiO5. This product usually appears as thin lath-like prisms showing parallel extinction, positive elongation and moderate birefringence. The crystals are optically positive with a fairly large optic angle. 2V = 68°. The indices of refraction are αNa = 1.614 ±.002, βNa = 1.620 ±.002, γNa = 1.633 ±.002. The optical plane is parallel to the macropinacoid (100) and the acute bisectrix Z is parallel to the direction of elongation which is taken as the crystallographic axis C. The optical properties and X-ray pattern are distinctive and entirely different from those of hillebrandite or foshagite, which have the same composition.Another crystalline calcium hydrosilicate was obtained by hydrothermal synthesis from excess lime and silica gel. This appeared as very small needle-like prisms, observable only when magnified about 200 times. The crystals show parallel extinction, positive elongation and very low birefringence with an index of refraction of 1.597 ±.003. Analysis of this product, extracted with a glycerol-water mixture to remove excess lime, gave a lime-silica ratio of 2 to 1 with an uncertain amount of water of at least one mole. The X-ray pattern is distinctive and shows only slight similarity to the hillebrandite pattern.