Single crystals of Ca0.9Nd0.1Ti0.9Al0.1O3 (CNTAO) were grown using optical floating zone technique and the grown crystals were characterized by Laue diffraction and powder X-ray diffraction techniques for crystal quality and its composition, respectively. The powder pattern of CNTAO was indexed and refined using GSAS program to an orthorhombic structure with space group Pbnm (#62), a = 5.3832(1), b = 5.4343(1), c = 7.6389(2) Å, V = 223.4677 Å3′, and Z = 4.