Variation in the martensitic transformation temperatures (TM) of quasi-ternary/off-stoichiometric Ni-Mn- Ga and Ni-Mn-Al-X alloys are correlated to their electron per atom ((e/a) ratios. The behavior of Fesubstituted Ni-Mn-Ga alloys is, however, anomalous. We use Pauling’s ideas on electronic structure of elements, and compute the number of non-bonding electrons (en)...