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In this paper, the pole figures plotted from X-ray diffraction data are employed to analyze the orientation of hydroxyapatite in ivory and mammoth ivory for the first time. The results present evidence of the lamellar structure and the hydroxyapatite appeared as tabular. A preferred orientation of hydroxyapatite was revealed in terms of the calculated orientation factor and the characteristics found in the pole figures. The c-axes of hydroxyapatite are mainly oriented along the growth direction. Both a-axes are on the left of the angle bisector of Retzius. Approximately 25–30° separates the a-axes and the angle bisector of Retzius in ivory, whereas the figure is approximately 10–15° in mammoth ivory. Our work is significant in providing more accurate knowledge of the shapes and organizational state of bio-mineral crystals and providing insight into crystal formation and development in bio-mineralization.