Ba(MoO4)x(WO4)1−x (x=0; 0.05; 0.1; 0.25; 0.5; 0.7; 0.95; 1) single crystals were grown by the Czochralski technique for the first time. A complete mutual solubility of the entire solid solution concentration range with tetragonal scheelite structure at room temperature was established by XRD analysis and Raman spectroscopy of as-grown crystals. By comparison of the differential-thermal analysis data and the high temperature Raman spectra, the existence of a cubic α-modification of the solid solutions is identified at x>0.5 in the temperature region above 1200°С. The double-mode behavior of the ν1(Ag) band in the vibration spectrum, weak broadening and high peak cross section of the ν1(Ag) vibration modes make these single crystals a promising material for dual-line SRS-conversion with a Raman shift of 889 and 925cm−1.