As the laser spot size in microscale laser shock peening is in the order of magnitude of several microns, the anisotropic response of grains will have a dominant influence on its mechanical behavior of the target material. Furthermore, conventional plasticity theory employed in previous studies needs to be re-examined due to the length scale effect. In the present work, the length scale effects in microscale laser shock peening have been investigated. The crystal lattice rotation underneath the shocked surface was determined via electron backscatter diffraction. From these measurements, the geometrically necessary dislocation (GND) density that the material contains has been estimated. The yield strength increment was then calculated from the GND distribution by using the Taylor model and integrated into each material point of the finite element method (FEM) simulation. Finite element simulations, based on single crystal plasticity, were performed for the process both with and without considering the GND hardening, and the comparison has been conducted.