In this study, a crystal plasticity finite element method (CPFEM) model has been developed to investigate the anisotropic plastic behavior of (001) aluminum single crystal during high-pressure torsion (HPT). The distributions of equivalent plastic strain and Mises stress recorded on the sample surface are presented. The directional variations of plastic strain and Mises stress with the development of four-fold symmetry pattern are observed along the sample circumference. The crystallographic orientation evolution along the tangential direction is studied, and the corresponding lattice rotation and slip trace are predicted, respectively. The plastic anisotropy mechanism is discussed in detail based on the theory of crystal plasticity. The simulation results reveal that the differences in slip systems activation (dominant slip and multiple slips) are responsible for the anisotropic plastic deformation in HPT.