A crystal plasticity model that can describe the complex work-hardening behavior and a homogenization method that is both accurate and computationally inexpensive are required for crystal plasticity-based sheet metal forming simulations. This study investigated several crystal plasticity models and homogenization methods for linear and nonlinear strain paths. In the experiments, the work-hardening behavior of an A5083-O sheet was measured under reverse and cross loadings. The anisotropy of the flow stress and plastic strain path was also measured in uniaxial tension and biaxial stress tests. The biaxial stress test included tension–tension and tension–compression combined stress states. The experimental and simulation results showed that the proposed crystal plasticity model accurately predicted the work-hardening behavior and texture evolution of the specimen. Furthermore, the two-grain cluster-type homogenization method captured the plastic anisotropy of the specimen as accurately as the finite element-based homogenization method. The computational speed of the two-grain cluster model was approximately 250 times faster than that of the finite element-based homogenization method. Therefore, the two-grain cluster model in conjunction with the proposed crystal plasticity model is an effective approach to predict the plastic behavior of polycrystals in large-scale sheet metal forming simulations.