The effects of Al substitution for Fe on the structure, magnetics, magnetostriction, anisotropy and spin reorientation of a series of Tb 0.3 Dy 0.6 Pr 0.1 (Fe 1−x Al x ) 1.95 alloys (x=0. 05, 0.1, 0.15, 0.2, 0.25, 0.3) at room temperature have been investigated. The alloys of Tb 0.3 Dy 0.6 Pr 0.1 (Fe 1−x Al x ) 1.95 substantially retain MgCu 2 -type C-15 cubic Laves phase structure when x<0.2. The mixed phases appear with x = 0.2, and cubic Laves phase decreases with increasing x. The magnetostriction of the Tb 0.3 Dy 0.6 Pr 0.1 (Fe 1−x Al x ) 1.95 alloys decreases drastically with increasing x and the giant magnetostrictive effect disappears for x > 0.15. Fortunately, a small amount of Al substitution is beneficial to a decrease in the magnetocrystalline anisotropy. The spin reorientation temperature decreases with increasing x. The analysis of the Mössbauer spectra indicates that the easy magnetization direction in the {110} plane deviates slightly from the main axis of symmetry with the increase of Al concentration x, namely, spin reorientation, resulting in the change of macroscopical magnetic properties and magnetostriction. The hyperfine field decreases, but the isomer shifts increases with Al concentration increasing and the quadruple splitting QS shows a weak concentration dependence. cubic laves phase, magnetostriction, spin reorientation, Mössbauer PACS: 75.80.+q, 76.80.+yThe pseudobinary rare-earth iron alloy Tb 0.3 Dy 0.7 Fe 2 (commercially known as Terfenol-D) as an excellent magnetostrictive material can be used as ultrasonic transducers and micro-actuators with giant magnetostrition and relatively low magnetocrystalline anisotropy [1]. However, its application is somewhat limited because of its low tolerance to tensile and shear forces, low electrical resistivity and relatively high saturation field. Many research works have focused on substituting Fe with other elements in an attempt to improve the magnetic and magnetostrictive properties in the Tb 0.3 Dy 0.7 (Fe 1−x T x ) 2 (T= Mn, Co, Ni, Ga, Al, B, Be, etc. ) alloys [2][3][4][5] and also to improve its application properties.Judging by these research reports, Al is regarded as an ideal substitution for Fe. The application properties of Tb 0.3 Dy 0.7 (Fe 0.9 Al 0.1 ) 1.95 alloys turn out excellent [5-9] because the addition of Al to Fe increases resistivity and ductility and decreases anisotropy, but its saturated magnetostriction greatly decreases. On the basis of retaining the good application properties, we anticipate that substitution of other elements for Tb or Dy enhances the saturated magnetostriction of Tb 0.3 Dy 0.7 (Fe 0.9 Al 0.1 ) 1.95 alloys.Pr is chosen as an ideal substitute for Fe among the numerous rare earth elements because the single ion model [1,10] indicates that the magnetostriction of PrFe 2 (λ 111 =5600 ppm) is larger than that of TbFe 2 (λ 111 =4400 ppm), DyFe 2 (λ 111 =4200 ppm) and SmFe 2 (λ 111 =−3200 ppm) at 0 K. Furthermore, the sign of magnetostriction of TbFe 2 , DyFe 2 and PrFe 2 is the same, but the sign of anis...