Fe 50 Ni 28 Co 17 Al 11.5 Ta 2.5 single crystals oriented along the [001] direction were investigated in order to establish the influence of two-step aging conditions on superelastic properties. The homogenized and quenched single crystalline material was subjected to a combination of high-temperature and low-temperature heat treatment at 973 K for 0.5 h and at 723 K for various aging times, respectively. As a result, fine and coherent γ' precipitates were formed. Using diffraction of high energy synchrotron radiation, the volume fraction of γ' precipitates was computed while their size was determined by high resolution TEM analysis. Compared with one-step heat treatment, the two-step aging process enables control of the precipitate size in a more accurate way. Moreover, it allows one to obtain a higher volume fraction of precipitates without increasing their size significantly. The obtained coherent γ' precipitates ranged in size from 5 to 8 nm; that considerably improved mechanical properties. The highest superelastic response was obtained for single crystals aged at 973 K for 0.5 h followed by aging at 723 K for 3 h. The single crystals treated with such conditions exhibited a superelastic strain of 15% in which the mechanical martensite stabilization was substantially suppressed.