New Raman spectroscopy data of mixed compounds in the row of compositions Li2Ca1-xSrxSiO4 where: x = 0 and 0.01, were obtained. The combined sol-gel method was used demonstrating the simplicity of complex compound synthesis with simultaneous rare-earth ion doping. High crystalline perfection of the synthesized materials with a small amount of optically neutral impurity in the presented polycrystalline materials was demonstrated by the X-ray structural analysis method. Using Raman spectroscopy and optical microscopy methods it was additionally proven that the main synthesized phase crystallizes with high structural perfection in the form of large individual crystallites. In the work, it was shown that the use of the Raman spectroscopy made it possible to exclude using complex expensive material analysis methods, such as synchrotron methods, in lithium-containing silicate systems. #COMESYSO1120.