A dislocation-density based crystalline plasticity (DCP) and nonlinear finite element (FE) analysis were used to predict, and fundamentally understand how and why fracture nucleation and propagation are related to the interrelated microstructural mechanisms of dislocation-density pileups, GB structure, orientation, and total and partial dislocation density interactions within and adjacent for a random low angle grain boundary (LAGB) and a random high angle GB (HAGB). The GB orientations and structures were obtained from micropillar experiments, such that LAGBs and the HAGBs can be accurately represented and used for the modeling predictions. The normal stress, density of pileups, and dislocation-density accumulation along and within the GB were higher for the low angle GB bicrystal. These interrelated phenomena delineate how fracture for high angle GBs nucleate and propagate at lower nominal strains than the lower angle GB bicrystal case. These predictions underscore how fundamental mechanisms can be identified and used to understand how failure nucleates and propagates for different GB structures and orientations.© 2024. The Author(s).