The pre-existing twin boundaries play an important role in the mechanical behaviors of metals. In the present work, we studied the bending deformation of [100]-oriented α-Fe nanowires seeded with 〈111〉/{112} twin boundaries using atomistic simulations. Bending behaviors along two different orientations were investigated. The initially flat twin boundaries become curved with a high density of 1/6 〈111〉/{112} partial dislocations under bending when the neutral plane intersects with twin plane along [01-1] direction, whereas could transform to the nonconventional {110} interfaces under bending when the neutral plane intersects with twin plane along [111] direction. The bent α-Fe nanowires could recover to the original state upon unloading, leading to a unique pseudoelasticity. The driving force for shape recovery primarily arises from the high interfacial energy, i.e. curved {112} twin boundaries or the transformed {110} interfaces. We further characterized the recoverability by the ratio η of the nanowire size (external length scale) to twin boundary spacing (internal length scale). This η-dependent recoverability matches well with the experimental data at large length scale. The present work may help understand the unique mechanical properties associated with twin boundaries in metals.