Piezoelectric crystals Ca3Nb(Al0.5Ga0.5)(3)Si2O14 (CNAGS) with langasite structure have been successfully grown by Czochralski method. In this work, the crystal structure, quality, chemical composition, piezoelectric properties, electric resistivity and optical properties of the as-grown crystals were characterized. The full width at half-maximum (FWHM) of the rocking curve of CNAGS was found to be 23 ''. The chemical compositions of CNAGS crystals are very close to that of initial compositions. At room temperature, the piezoelectric coefficients d(11) and d(14) of CNAGS crystals are 4.12 pC/N and -5.03 pC/N, and the electromechanical coupling coefficients k(12) and k(26) are also determined as 11.6% and 18.3%, respectively. The electric resistivity of as-growth crystal was found to be on the order of 2 x 10(8) Omega cm at 500 degrees C and 1 x 10(6) Omega cm at 800 degrees C. And the transmittances of CNAGS crystals were found to be over 80% in the wavelength range of 700-2700 nm.