Fe-Mn-Al-Ni shape memory alloy (SMA) is a promising candidate because of its lower cost and better cold-workability compared with Ti-Ni alloy [1]. This alloy is attractive for large components, for example, in civil engineering applications. There are two important features of this alloy system. The first one is the small temperature dependence of critical stress for martensitic transformation, which allows this superelastic alloy to be used in a wide temperature range. The other one is easy fabrication of single crystal through abnormal grain growth (AGG) induced by the cyclic heat treatment. Recently, we have discovered that the temperature dependence of critical stress in this alloy can be tuned from a positive to a negative value by adding Cr [2]. Besides, near-constant critical stress temperature dependence is obtained with 3 to 4 at.% Cr, and this behavior is highly desirable for applications that involve large temperature fluctuations. Since the superelastic performance in this alloy system is closely related to the BCC phase stability and NiAl precipitates, in this study, the effect of Al and Cr contents on the superelastic performance in Fe-Mn-Al-Ni superelastic alloys was investigated.