The effect of Al substitution for Fe on crystal structure, magnetostriction and spontaneous magnetostriction, anisotropy and spin reorientation of a series of polycrystalline Tb 0.3 Dy 0.7 (Fe 1−x Al x ) 1.95 alloys (x = 0, 0.05, 0.1, 0.15, 0.20, 0.25, 0.30, 0.35) at room temperature and 77 K was investigated systematically. It was found that the primary phase of Tb 0.3 Dy 0.7 (Fe 1−x Al x ) 1.95 is the MgCu 2 -type cubic Laves phase structure when x < 0.4 and the lattice constant a of Tb 0.3 Dy 0.7 (Fe 1−x Al x ) 1.95 increases approximately and monotonically with the increase of x. The substitution of Al leads to the fact that the magnetostriction λ inceases slightly in a low magnetic field (H ≤ 40 kA/m), but decreases sharply and is easily close to saturation in a high applied field as x increases, showing that a small amount of Al substitution is beneficial to a decrease in the magnetocrystalline anisotropy. It was also found that the spontaneous magnetostriction λ 111 decreases greatly with x increasing. The analysis of the Mössbauer spectra indicated that the easy magnetization direction in the {110} plane deviates slightly from the main axis of symmetry with the changes of composition and temperature, namely spin reorientation. A small amount of non-magnetic phase exists for x = 0.15 in Tb 0.3 Dy 0.7 (Fe 1−x Al x ) 1.95 alloys and the alloys become paramagnetic for x > 0.15 at room temperture, but at 77 K the alloys still remain magnetic phase even for x = 0.2. At room temperature and 77 K, the hyperfine field decreases and the isomer shifts increase with Al concentration increasing.