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Crystallization behavior of amorphous chenodeoxycholic acid (CDCA) was studied using X-ray diffraction (XRD), infrared (IR) spectroscopy and differential scanning calorimetry (DSC). The two polymorphs of CDCA, form I (mp 166 °C) and form III (mp 119 °C), were ground with a vibrational mill. The ground samples of both crystal forms showed halo X-ray diffraction patterns. DSC curves of the amorphous samples derived from the form I and form III showed exothermic peaks due to the crystallization to the form I at 120 and 147 °C, respectively. When the ground form III was mixed with the ground form I, the crystallization temperature shifted to a lower temperature as the content of the ground form I increased. In the case of co-ground sample of form I and form III, the crystallization to form I crystals proceeded by two different modes. These results indicate that the physicochemical state was different among the ground samples of the form I and form III, and that the crystal nuclei played an important role on the crystallization process of the amorphous CDCA.