Newly developed polymer infiltrated grain aligned composite Terfenol-D has the advantages of maintaining the favorable crystal orientation of the directionally grown RFe2 phase. In order to infiltrate the polymer effectively, it is necessary to prepare composition with a low Fe content (0.64 less than or equal to y less than or equal to 1.7) in Tb0.33Dy0.67Fey. With decreasing Fe content, the amount of the eutectic phase increases which can be removed by annealing. This composite shows many improved properties compared with conventional composite or monolithic Terfenol-D material. Through this new material, high magnetostrictive strain can be obtained under relatively low magnetic field. In addition, it shows a considerably higher modulus of rupture of around 65similar to92 MPa in four-point bend test.