Growth of 2-in. diameter Al-substituted Ca3TaGa3Si2O14 crystals by Czochralski method is reported. The crystals were grown from the melt of Ca3TaGa1.5Al1.5Si2O14 composition and had langasite structure. No inclusions of secondary phases were detected in these crystals. The Ca3Ta(Ga,Al)(3)Si2O14 mixed crystals produced using non-substituted Ca3TaGa3Si2O14 seeds were defective. They had cracks and/or polycrystalline structure. However, those grown on the seed of approximately Ca3TaGa1.5Al1.5Si2O14 composition were defect-free. Phase diagram of the Ca3TaGa3Si2O14-Ca3TaAl3Si2O14 pseudo-binary system and segregation phenomenon are discussed in some details. Homogeneity of the crystals was evaluated by measuring 2D-mapping of leaky surface acoustic wave (LSAW) velocities for Y-cut Ca3TaGa1.5Al1.5Si2O14 substrate. Although some inhomogeneities were observed due to slight variations in chemical composition, the crystal had acceptable homogeneity for applications in acoustic wave devices exhibiting the LSAW velocity variation within +/- 0.048%. (C) 2016 Elsevier B.V. All rights reserved.