We combine chelate-assisted solvent extraction (CASE) and hot hydrogen fluoride gas treatment to enable a general method for the preparation of high-purity binary metal fluorides. The fluorozirconate glass ZBLANI:Yb(3+) (ZrF(4)-BaF(2)-LaF(3)-AlF(3)-NaF-InF(3)-YbF(3)), a solid-state laser-cooling material, is used as a test case to quantitatively assess the effectiveness of the purification method. The reduction of transition-metal and oxygen-based impurities is quantified directly by inductively coupled plasma mass spectrometry (ICP-MS) and indirectly by laser-induced cooling, respectively. The concentrations of Cu, Fe, Co, Ni, V, Cr, Mn, and Zn impurities in the ZrCl(2)O precursor solution were measured individually by ICP-MS at various stages of the purification process. CASE was found to reduce the total transition-metal concentration from 72500 to similar to 100 ppb. Laser cooling was most efficient in ZBLANI:Yb(3+) glass fabricated from CASE-purified metal fluoride precursors, confirming the results of the ICP-MS analysis and demonstrating the effectiveness of the purification methods in a finished optical material. High-purity metal fluorides prepared by the methods presented herein will enable new high-performance optical materials for solid-state optical refrigerators, crystals for vacuum ultraviolet (VUV) spectroscopy of the Thorium-229 nucleus, VUV optics, fibers, and thin-film coatings.