The solubility of Ba(NO3)2 and Sr(NO3)2 crystals in aqueous solution from 25 to 65°C has been determined by both an optical interferometer and a weight technique. A Mach-Zehnder interferometer was used for measuring the concentration distribution of Ba(NO3)2 and Sr(NO3)2 near the solid/liquid interface during crystal growth and dissolution. A fringe carrier technique was introduced to visualize more clearly the boundary layer and to solve the concentration distribution. Crystals were successfully grown with sizes larger than 60mm×60mm×70mm by a temperature cooling method. The BaxSr1−x(NO3)2 crystal was also nucleated and grown. The Raman spectra of BaxSr1−x(NO3)2 indicate that the barium ions probably degrade the properties of Sr(NO3)2.