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Plate-impact experiments were conducted to study the features and mechanisms of void nucleation and growth in the polycrystalline of pure aluminum under dynamic loading. Soft-recovered samples have been analyzed by metallographic microscopy, electron back scattering diffraction (EBSD), and synchrotron radiation x-ray tomography technology. It was found that most of the void nucleation in grains neared the boundaries of “weak-orientation” grains and grew toward the grain boundaries with fractured small grains around the boundaries. This was mainly caused by the accumulation and interaction of slip systems in the “weak-orientation” grains. In addition, the micro voids were nearly octahedron because the octahedral slip systems were formed by 8 slip planes in the polycrystalline of pure aluminum. The EBSD results are consistent with the three-dimensional structure observed by synchrotron radiation x-ray.