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Mn–Cu-based damping alloy prepared by directional solidification is very promising for vibration and noise control. Aging treatment with and without application of magnetic field on the microstructure and damping performance of directionally solidified Mn–Cu alloy was studied by means of X-ray diffraction, differential scanning calorimetry, dynamic thermal mechanical analysis and scanning electron microscope. It is found that aging treatment makes the orientation shift from (200) to (111), and aging treatment under magnetic field helps Mn–Cu alloy keep high damping in the wide temperature range. The polymorphic microstructure characterised by fine twin bands with low-angle misorientation boundaries leads to a substantial increase of twin boundary internal friction up to several times higher than that of polycrystalline state.