Platelet-like kassite, a rare mineral CaTi2O4(OH) 2, was synthesized by a wet chemical route using Ca(OH)2 and TiO2 as reagents in base solution. The microstructure of the obtained kassite examined by synchrotron radiation and Rietveld refinement are hexagonal (P312) with a = b = 0.52451(2) and c = 0.47844(3) nm. This cell is slightly different from JCPDS No. 88-1722. At heating above 500 °C, the layered crystalline kassite rearranges to form, disk-like CaTiO3 and amorphous TiO2 by removing H2O completely. Furthermore, transmission electron microscopy analysis reveals that the vertical axis of disk-like CaTiO3 along the  direction converts from that of  of kassite.