The activated slip systems were analyzed in the cold rolling of a Ni₃Al single crystal with an initial orientation of ~[-112](512), which showed an irregular rolling deformation, i.e. widening, bending, and shear deformation. A phenomenological crystal plasticity model was applied using a spectral method. The boundary condition was optimized to reproduce the actual rolling deformation, as follows. That is, the orthogonal components of the deformation gradient were given from the measured widening and reduction, and the shear components were iteratively optimized as to that the final orientation was as close to the experimental one as possible. The calculated result showed that three slip systems, a3, b1, and d1 in the Bishop-Hill notation, were mainly activated in the irregular rolling deformation, which result was consistent to the previous observation of the slip traces [Kishida et al., Philos. Mag. 83 (2003) 3029]. The three activated systems were identical to those activated in the plane-strain condition. However, the quantitative comparison revealed that the activity of b1 was significantly reduced in the irregular rolling deformation, while the activity of d1 was enhanced instead. The less activity of b1 and the enhancement of d1 can be understood assuming a strong interaction between a3 and b1. The reaction of this pair has been reported to form the superlattice intrinsic stacking fault (SISF) in Ni₃Al [Chiba and Hanada, Philos. Mag. A. 69 (1994) 751]. It is likely that the formation of the SISF, which are considered immobile in Ni₃Al, restrained the activation of b1, leading to the irregular rolling deformation.