Pseudoelasticity in Fe 3 Al single crystals with the D0 3 structure was investigated focusing on the ordering process and the ordered domain structure. During unloading, a plastic strain of 5.0% was perfectly recovered in Fe-23.0at.%Al single crystals with an appropriate heat treatment, while Fe-28.0at.%Al crystals exhibited little strain recovery. The ordered domain structures in slowly cooled Fe-23.0at.%Al and Fe-28.0at.%Al were different from each other depending on their ordering process. In Fe-23.0at.%Al, the strong interaction between specific domain boundaries and superpartial dislocations with Burgers vector of 1/4<1 1 1> led to the individual motion of the superpartials dragging an antiphase boundary (APB). The surface tension due to the APB resulted in the pseudoelasticity in Fe-23.0at.%Al single crystals. In addition, APB created by an intersection between the domain boundaries and the superpartials also pulled back the superpartials during unloading. A refinement of ordered domains was effective in enhancing the pseudoelasticity in Fe 3 Al crystals.