The effect of Ga content on the actuation behavior, i.e., λ(magnetostriction)—H and B—H curves, of single-crystal iron-gallium (FeGa) is studied by characterizing 19, 24.7, and 29 at.% Ga 〈100〉 oriented slow cooled samples. The strikingly different behavior exhibited by these samples is discussed and explained in this study. In an attempt to understand the effect of crystallographic direction on the magnetomechanical behavior, the actuation and sensing, i.e., ε(total strain)—σ and B—σ characterization of both a 〈100〉 oriented 19 at.% Ga sample and 〈110〉 oriented 18 at.% Ga is performed, and is presented and analyzed. Furthermore, a testing paradigm that has been developed to characterize the sensing behavior independent of the magnetic interaction between the magnetostrictive sample and the magnetic bias circuit is discussed.