Pure C₆₀ single crystals were grown by a sublimation-condensation method in an evacuated closed quartz tube situated in a double-temperature-gradient furnace. Large C₆₀ single crystals, up to a size of 0.6 mm × 1.0 mm × 2.0 mm with quite smooth and shiny faces, were obtained. X-ray diffraction, electron diffraction and x-ray morphology were carried out and showed that the quality of large C₆₀ single crystals grown by the double-temperature-gradient technique is excellent. In this paper the experimental results of the growth of large C₆₀ single crystals are reported and the morphological and structural characterizations are discussed in detail.