Iron is a well-utilized material in structural and magnetic applications. This does not mean, however, that it is well understood, especially in the field of magnetostriction. In particular, the rhombohedral magnetostriction of iron, λ111 , is anomalous in two respects: it is negative in sign, in disagreement with the prediction of first principles theory, and its magnitude decreases with increasing temperature much too rapidly to be explained by a power law dependence on magnetization. These behaviors could arise from the location of the Fermi level, which leaves a small region of the majority 3d t2g states unfilled, possibly favoring small internal displacements that split these states. If this view is correct, adding small amounts of Co to Fe fills some of these states, and the value of λ111 should increase toward a positive value, as predicted for perfect bcc Fe. We have measured the magnetostriction coefficients (λ111 and λ100) of pure Fe, Fe97Co3, and Fe94Co6 single crystals from 77 K to 450 K. Resonant ultrasound spectroscopy has been used to check for anomalies in the associated elastic constants, c 44 and c′. The additional electrons provided by the cobalt atoms indeed produced positive contributions to bothmagnetostriction constants, λ111 and λ100, exhibiting an increase of 2.8 × 10−6 per at. % Co for λ111 and 3.8 × 10−6 per at. % Co for λ100.