A microstructural informed thermodynamic model is utilized to tailor the pseudoelastic performance of a series of Fe–Mn–Al–Ni shape‐memory alloys. Following this approach, the influence of the stability and the amount of the B 2‐ordered precipitates on the stability of the austenitic state and the pseudoelastic response is revealed. This is assessed by a combination of complementary nanoindentation measurements and incremental‐strain tests under compressive loading. Based on these investigations, the applicability of the proposed models for the prediction of shape‐memory capabilities of Fe–Mn–Al–Ni alloys is confirmed. Eventually, these thermodynamic considerations enable the guided enhancement of functional properties in this alloy system through the direct design of alloy compositions. The procedure proposed renders a significant advancement in the field of shape‐memory alloys.