The process of laser shock peening induces compressive residual stresses in a material to improve material fatigue life. For micron sized laser beams, the size of the laser-target interaction zone is of the same order of magnitude as the target material grains, and thus the target material must be considered as being anisotropic and inhomogeneous. Single crystals are chosen to study the effects of the anisotropic mechanical properties. It is also of interest to investigate the response of symmetric and asymmetric slip systems with respect to the shocked surface. In the present study, numerical and experimental aspects of laser shock peening on two different crystal surfaces (110) and of aluminum single crystals are studied. Lattice rotations on the top surface and cross section are measured using electron backscatter diffraction, while residual stress is characterized using X-ray microdiffraction. A numerical model has been developed that takes into account anisotropy as well as inertial terms to predict the size and nature of the deformation and residual stresses. Obtained results were compared with the experimental finding for validation purpose.