Fe1−xMx (M = Ga, Ge, Si, Al, Mo and x ∼ 0.18) alloys offer an extraordinary combination ofmagnetoelasticity and mechanical properties. They are rare-earth-free, can be processed using conventional deformation techniques, have high magnetic permeability, low hysteresis, and low magnetic saturation fields, making them attractive for device applications such as actuators and energy harvesters. Starting with Fe-Ga as a reference and using a rigid-band-filling argument, Zhang et al. predicted that lowering the Fermi level by reducing the total number of electrons could enhance magnetoelasticity. To provide a direct experimental validation for Zhang's hypothesis, elemental additions with lower-than-Ga valence are needed. Of the possible candidates, only Be and Zn have sufficient solubility. Single crystals of bcc Fe-Ga-Zn have beengrown with up to 4.6 at. % Zn in a Bridgman furnace under elevated pressure (15 bars) in order to overcome the high vapor pressure of Zn and obtain homogeneous crystals. Single-crystalmeasurements of magnetostriction and elastic constants allow for the direct comparison of themagnetoelastic coupling constants of Fe-Ga-Zn with those of other magnetoelastic alloys in its class. The partial substitution of Ga with Zn yields values for the magnetoelastic coupling factor, −b 1, comparable to those of the binary Fe-Ga alloy.