Dislocation substructure in NiAl single crystals oriented for single slip and deformed at ambient temperature has been studied using weak-beam transmission electron microscopy. Deformation is localized in bands that consists mostly of near-edge dislocations, with an interspersion of a high density of elongated prismatic loops. Pure screw dislocations ate not observed, but dislocations having ''zigzag'' configurations that are near-screw in orientation are present. A high density of jogs is observed on both near-edge and zigzag dislocation segments. The mechanisms for the development of this substructure are discussed, emphasizing the role of double cross slip and resulting glissile and sessile jogs of varying heights.