This study systematically investigated the effect of Mo addition on the microstructure and superelasticity of Fe-Mn-Al-Ni alloy. The findings indicate that the addition of Mo element efficaciously suppressed the formation of γ phase after air cooling. Single crystal samples were prepared through cyclic heat treatment. The size of the precipitates in the solid-solution single crystal was found to be ∼ 12.90 nm. In contrast, the mean precipitates size in the aging single crystal was ∼ 18.07 nm. An excellent superelasticity with an average recoverable strain of ∼ 8 % at an applied strain of ∼ 9.5 % can be obtained in both the solid solution and aging single crystals with a near [-412] orientation. The Mo addition widens the size range of precipitates with good superelasticity up to ∼ 18 nm. Additionally, there is a significant difference in the superelastic performance of single crystals with different orientations. Superelastic strain values for orientated single crystals near [-412], [1-20] and [‐14‐3] were 5.5 %, 4.8 % and 4.4 %, respectively.