Langasite (La3Ga5SiO14, LGS) and its isomorphs, were regarded as potential substrate materials for surface acoustic wave (SAW) and bulk acoustic wave (BAW) applications. Among these homologous compounds, the ordered structure crystals have attracted much attention for their low Ga2O3 content, high acoustic velocity and low acoustic loss. In this work, the ordered langasite structure crystals Ca3NbGa3Si2O14 (CNGS) were grown with vertical Bridgman method for the first time. The CNGS crystals with 25mm in diameter and 40mm in length were grown successfully from its stoichiometric melt through LGS crystal of Ø10mm×40mm being chosen as seed. X-ray powder diffraction experiments showed that the CNGS single crystals had a single phase and had the same structure as the LGS crystal. The transmittance spectra with the wavelength from 200 to 800nm were recorded by means of Spectrophotometer at room temperature.