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Measured 57Fe-isomer shifts for face-centered cubic FeyNi1−y alloys show a linear variation with ∂1S/∂y = +0.10 mm s−1 up to [Formula: see text] followed by a plateau at [Formula: see text], up to the structural stability limit at [Formula: see text]. This is in disagreement with recent ab initio calculations, however, the increase at [Formula: see text] is in quantitative agreement with an older modified tight-binding approach in which the increase arises from an atomic volume dependence. The plateau is an anomaly that sets in at the same composition as that at which the saturation moments start to deviate from the Slater–Pauling curve.