Compression tests at low strains were performed to theoretically analyze the effects of anisotropic elasticity, misorientation, grain boundary (GB) stiffness, interfacial dislocations, free surfaces, and critical force on dislocation pile-ups in micro-sized Face-Centered Cubic (FCC) Nickel (Ni) and α -Brass bi-crystals. The spatial variations of slip heights due to localized slip bands terminating at GB were measured by Atomic Force Microscopy (AFM) to determine the Burgers vector distributions in the dislocation pile-ups. These distributions were then simulated by discrete pile-up micromechanical calculations in anisotropic bi-crystals consistent with the experimentally measured material parameters. The computations were based on the image decomposition method considering the effects of interphase GB and free surfaces in multilayered materials. For Ni and α -Brass, it was found that the best predicted step height spatial profiles were obtained considering anisotropic elasticity, free surface effects, a homogeneous external stress and a certain critical force in the material to equilibrate the dislocation pile-ups.