This work combined experiments at the grain level with the constitutive modeling of a single crystal to investigate deformation behaviors of a pure aluminum single crystal oriented for a single slip. Simple compression of a [132] single crystal was conducted to obtain the macroscopic stress—strain response and observe the deformed shape of the sample. The evolution of the crystallographic orientation was measured by an electron backscattered diffraction system in a field emission scanning electron microscope. The heterogeneous in-plane surface deformation in a single crystal was calculated by using a digital image correlation technique. Finite element modeling based on a single crystal plasticity model agrees well with experimental results in an averaged sense, not at the individual dislocation level.