The mechanical properties and dislocation microstructure of single crystals with a range of compositions within the Fex-Ni60–x-Al40 pseudobinary system have been investigated, with the purpose of bridging the behavior from FeAl to NiAl. Experiments are focused on the compression testing of <001> oriented single crystals with compositions where x = 10, 20, 30, 40, and 50 (in atomic percent). Observations of a<111> dislocation morphologies at room temperature and both a<111> and non-a<111> dislocation activity at elevated temperatures are reported and discussed. Measurements of the yield strength, elastic modulus and strain hardening rates are reported, and the variation of strength with composition is correlated with dislocation dissociation and overall dislocation morphology.