Vibratory power generation technology using the inverse magnetostriction effect, which is a magnetic flux change induced by stress, in ferromagnetic materials has attracted significant attention. Recently, polycrystalline magnetostrictive alloys with a combination of high stiffness and strength and large magnetostriction have become desirable for various smart applications, such as energy harvesters [1] and microscale sensors [2] and actuators. [3] However, the current understanding of the microstructure-property relationship of magnetostrictive materials is still limited due to the complexity of their grain geometry, multi-objective design requirements, and the lack of experimental verifications. [4,5] In 1965, Clark et al. [6] reported that Tb-Dy-Fe alloy (Terfenol-D) exhibits excellent magnetostriction (%1600 ppm), a large generated force (%30 000 N), and high responsiveness (%40 μs). Magnetostrictive alloys have been widely used as actuators, but the scope of engineering applications is limited because of the brittleness in Terfenol-D. In 2000, Fe-Ga-Al alloy (Galfenol) attracted attention for its excellent magnetostrictive properties and rigidity. [7-10] Many studies focus on the addition of third elements or controlling the nanostructure. Wu et al. [11] reported that the addition of the rare-earth element Tb exhibited large magnetostriction (400 ppm) and good strength (400 MPa). Recently, Na et al. [12] developed Fe-Al alloy (Alfenol) with a strong <100> orientation in the roll direction that showed good magnetostriction (%200 ppm) and tensile strength (606 MPa). Thus, it is speculated that the magnetostriction and mechanical properties of magnetostrictive materials show a contradictory relationship; that is, there are some difficulties in improving both characteristics simultaneously. Mashiyama [13] and Furuya et al. [14] found that Co-rich Fe 1-x Co x alloys (x ¼ 50-90 at%) have excellent magnetostrictive and mechanical properties. [15-18] Yamaura et al. [19] demonstrated larger magnetostriction of 128 ppm along the rolling direction in an Fe 25 Co 75 alloy by cold rolling (rolling rate of %97%) compared with the other composition in Fe-Co system. These Co-rich Fe-Co alloys have been gradually used commercially because they are easy to transform into any shape for applications. [20-25] Thus, the composition of Fe 29 Co 71 seems to be superior to the other composition in the viewpoint of magnetostrictive and mechanical characteristics in Fe-Co system. [13,19] These characteristics are preferred to be the applications of mechanical sensors or energy harvesters assumed in an industrial environment.