Micromechanism of crystal growth has received considerable attention as a fundamental subject. However, in situ observation of the crystal growth process remains challenging. In this study, high-temperature Raman spectroscopy has been utilized to investigate the growth pattern of Bi2ZnOB2O6 crystals via in situ exploration of the starting solution structure near the crystal-solution interface. The experimental results show that the solution primarily consists of ZO4 and BO3 units corresponding to 370, 539, 664, and 1293 cm-1 vibration frequencies. These units connect with each other forming longer chains in the area close to the crystal, and they are related to the presence of low-wavenumber vibrations in the Raman spectrum. Furthermore, a loose embryonic structure of the Bi2ZnOB2O6 crystal is observed near the crystal-solution interface owing to the formation of Bi-O bonds. Therefore, this study successfully provides a clear understanding of the formation mechanism of Bi2ZnOB2O6 crystals.