This article will review the development of the Fe-Ga (Galfenol) alloy system for magnetostriction applications including work on substitutional ternary alloying additions for magnetic property enhancement. A majority of the alloying addition research has focused on substitutional ternary elements in Bridgman grown single crystals with the intent of improving the magnetostrictive capability of the Galfenol system. Single crystals provide the ideal vehicle to assess the effectiveness of the addition on the magnetostrictive properties by eliminating grain boundary effects, orientation variations, and grain-to-grain interactions that occur when polycrystals respond to applied magnetic fields. In almost all cases, ternary additions of transition metal elements have decreased the magnetostriction values from the binary Fe-Ga alloy. Most of the ternary additions are known to stabilize the D0(3) chemical order and could be a primary contribution to the observed reduction in magnetostriction. In contrast, both Sn and Al are found to substitute chemically for Ga. For Sn additions, whose solubility is limited, no reduction in magnetostriction strains are observed when compared to the equivalent binary alloy composition. Aluminum additions, whose effect on the magnetoelastic coupling on Fe is similar to Ga, result in a rule of mixture relationship. The reviewed research suggests that phase stabilization of the disordered bcc structure is a key component to increase the magnetostriction of Fe-Ga alloys.