Transparent and pale yellow calcium barium niobaLes (CaxBa1-xNb2O5), single crystals with larger Ca content ranging from 0224 to 0.366 have been grown our by floating zone technique. The growth of CBN crystals in air is oriented along the < 001 > direction. The CBN crystals have been characterized by X-ray diffraction and X-ray single crystal diffraction. The composition uniformity of CBN-35 crystal rod has been checked by EPMA measurement. The deviations of Ca mole fraction between initial melt and the crystal are 0.1-1A mol%, which is much lower than crystals prepared by the Czochralski method, All the as grown crystals had high transmittance above 80% with increasing wavelength from about 500 nm. With increasing Ca content in crystal, symmetric bending mode 15 and symmetric stretching mode nu(2) broadened and moved to the low wave number. The relative intensity of Raman peak vs compared to nu(2) increasing gradually indicates that the NbO6 octahedral distortion degree increased. (C) 2014 Elsevier B.V. All rights reserved.