Alloys of Fe82Ga18−xAlx (x=0, 4.5, 6, 9, 12, 13.5) were prepared by directional solidification technique and exhibited a <001> preferred orientation along the axis of alloy rods. The saturation magnetostriction value of the Fe82Ga13.5Al4.5 alloy was 247ppm under no pre-stress. The tensile properties of alloys of Fe82Ga18−xAlx at room temperature were investigated. The results showed that tensile ductility of binary Fe-Ga alloy was significantly improved with Al addition. The fracture elongation of the Fe82Ga18 alloy was only 1.3%, while that of the Fe82Ga9Al9 alloy increased up to 16.5%. Addition of Al increased the strength of grain boundary and cleavage, resulting in the enhancement of tensile ductility of the Fe-Ga-Al alloys. Analysis of deformation microstructure showed that a great number of deformation twins formed in the Fe-Ga-Al alloys, which were thought to be the source of serrated yielding in the stress-strain curves. The effect of Al content in the Fe-Ga-Al alloys on tensile ductility was also studied by the analysis of deformation twins. It indicated that the joint effect of slip and twinning was beneficial to obtain the best ductility in the Fe82Ga9Al9 alloy.