The longitudinal magnetostriction of the [100] rod single crystals of iron containing 0.5%Al has been studied at ordinary temperatures, using the optical lever method, in the thermally demagnetized state and in the alternating-current demagnetized state. It has been found that the dependence of the magnetostrictive behaviors of these specimens on the method of demagnetization is more distinguished than that of the [100] single crystals of pure iron reported until now. Also, it has been determined quantitatively, from the magnetostriction vs. magnetization curves in the thermally demagnetized state, that the volume fraction of domains with magnetization vectors along the direction of easy magnetization nearest to the rod axis in the unmagnetized state ranges from 0.11 to 0.15, and that the value of the magnetostrictive constant, λ100, is 15.7×106. Furthermore, the deviation of the domain distribution in the state of remanent magnetization from that governed by Kaya’s rule has been evaluated.