A series of synthetic calcium silicates has been produced comprising nano-sized plates. The starting calcium silicate referred to as nano-structured calcium silicate, NCS, appears itself X-ray amorphous but contains impurities of calcite. These impurities decompose during the dry thermal conversion of the material into wollastonite. NCS can be enriched with calcium or silicon, respectively. The silicon enriched NCS can be hydrothermally transformed into a sheet material related to Ca7Si16O38(OH)2. The X-ray pattern of this material was sufficient to allow the calculation of its unit cell with a comparatively high figure of merit. The calcium enriched NCS can form two very distinctly different ceramic materials upon hydrothermal treatment, one a band material (formed below 200 °C) and the other a rose petal shaped material (formed above 210 °C). The X-ray diffraction patterns could not be resolved. The fit between the observed and calculated patterns was less than 50% as expressed in comparatively low figures of merit (unusually <20), which is attributed to calcium carbonate impurities in the samples disrupting the long range order. The patterns of these calcium enriched samples could be best compared to those of tobermorite or truscotite.