Texture and microstructure evolution during cold rolling of binary Nb3Al single crystals were studied as a function of the initial crystal orientations. Cold rolling behavior of the single crystals is strongly dependent on the initial crystal orientations, especially on the initial rolling direction (RD). Macroscopic texture evolutions for binary Ni3Al single crystals with the initial RD close to < 001 > are characterized as development of dual {110}< 112 > texture above 90% cold reduction and the banded structure formation. Microstructure observations reveal the extensive formation and accumulation of the planar defects including the stacking faults and the planes where the localized shear deformations occurs, which must be responsible for the observed anisotropic cold rolling behavior of Ni3Al single crystals.