The deformation behavior of aluminum single crystals subjected to compression along the [100] and [110] directions is numerically examined in terms of crystal plasticity. A constitutive model taking into account slip geometry in face-centered cubic crystals is developed using experimental data for the single-crystal samples with lateral sides coplanar to certain crystal planes. Two sets of calculations are performed using ABAQUS/Explicit to examine the features of plastic strain evolution in perfectly plastic and strain-hardened crystals. Special attention is given to the discussion of mechanical aspects of crystal fragmentation. Several distinct deformation stages are revealed in the calculations. In the first stage, narrow solitary fronts of plastic deformation are alternately formed near the top or bottom surfaces and then propagate towards opposite ends to save the symmetry of the crystal shape. The strain rate within the fronts is an order of magnitude higher than the average strain rate. The first stage lasts longer in the strain-hardened crystals, eventually giving way to an intermediate stage of multiple slips in different crystal parts. Finally, the crystal shape becomes asymmetrical, but no pronounced macroscopic strain localization has been revealed at any deformation stage. The second stage in perfectly plastic crystals relates to abrupt strain localization within a through-thickness band-shaped region, accompanied by macroscale crystal fragmentation. Stress analysis has shown that pure compression took place only in the first deformation stage. Once the crystal shape has lost its symmetry, the compressive stress in some regions progressively decreases to zero and eventually turns tensile.