T-x diagram of LiNO3-NaNO3 quasi-binary system has been improved using an original technique based on Raman measurements of condense phase. (LiNO3)(x)(NaNO3)(1-x) solid solution single crystal has been grown at different regimes of axial vibrational control (AVC) technique. Significant difference in segregation coefficient behavior between AVC-CZ and conventional CZ grown crystals has appeared: with AVC intensity increase the segregation coefficient (SC) raises for light molecular weight elements, SC reduces for medium molecular weight elements, and SC remains practically unchangeable for heavy molecular weight elements. Effect of vibrational intensity on vibron and optical characteristics, microhardness of AVC-CZ (LiNO3)(x)(NaNO3)(1-x) solid solution single crystals has been studied. For the AVC-CZ crystals has been observed increases in microhardness as well as in optical transmission up to 10 rel% compare to conventional CZ grown crystals. (C) 2014 Elsevier B.V. All rights reserved.