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Good quality benzimidazole (BMZ) single crystals were successfully grown by the vertical Bridgman technique (VBT). The unavoidable thermal-induced structural grain boundaries formed in the normal VBT growth of these crystals with low melting point were controlled by using a double-wall ampoule. The grown single crystals were subjected to high-resolution X-ray diffraction to assess their crystallinity. The enhancement of optical properties due to the improvement in crystalline perfection is also reported.