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The average magnetic moment and the magnetic moments of the sublattices of (Fe1–xMnx)3Al alloys are determined from saturation magnetization and neutron diffraction. By Mössbauer experiments the effective magnetic fields on 57Fe nuclei are measured. The distribution of Fe, Mn, and Al on the three sublattices of the DO3 structure are determined by means of neutron and X‐ray diffraction. The observed decrease of magnetic moments with increasing Mn concentration is explained by the occurrence of parasitic antiferromagnetism. Also 55Mn spin‐echo measurements show the existence of antiferromagnetically coupled magnetic moments.