Al-doped Ca3TaGa3Si2O14 single crystals with various Al concentrations were grown by the micropulling-down method and their structure and chemical composition were investigated. Ca3Ta(Gas(1-x)Al(x))3Si(2)O(14) crystals with x=0, 0.2, 0.4, 0.6, 0.8 and 1 were grown. They were highly transparent and a single phase of langasite-type structure was confirmed in the powder X-ray diffraction measurement. Their lattice parameters related to the a- and c-axes systematically decreased with increase in Al concentration. It followed from the EPIVIA analysis that the real Al concentration in the crystals almost corresponded to the nominal compositions. (C) 2014 Elsevier B.V. All rights reserved.