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Abstracts: Energetic materials have to face variable environments throughout their life cycle. Therefore, revealing the evolvement of energetic materials under complex conditions is of great importance for their applications. As an energetic material, α-2,4-Dinitroanisole (α-DNAN) exhibits low sensitivity and can be used in the formulation of melt-cast insensitive munitions as a replacement for TNT. Despite numerous studies focusing on DNAN, the high-pressure investigation of DNAN is still limited. Using diamond anvil cell and resistance heating techniques, this study investigates the structural variation and melting performance of α-DNAN at high pressures. The results are as follows. A phase transition occurred at 1.5 ​GPa. The high-pressure phase kept stable and had the tendency to be amorphous at high pressures. The high-temperature and high-pressure Raman measurement and optical photographing illustrated that pressure significantly influenced the melting temperature of α-DNAN. From 0.6 to 1.2 and then to 1.9 ​GPa, the melting point increased from 130 ​°C to 182 ​°C and finally to 285 ​°C. When the pressure reached 1.9 ​GPa, decomposition occurred and was accompanied by a melting process. This high-pressure and high-temperature study of DNAN contributes to deeply understanding the structural stability of DNAN and provides important data for the manufacture and storage of DNAN.