Evolving dislocation-density pile-ups at grain-boundaries (GBs) spanning a wide range of coincident site lattice (CSL) and random GB misorientations in face-centered cubic (fcc) bicrystals and polycrystalline aggregates has been investigated. A dislocation-density GB interaction scheme coupled to a dislocation-density-based crystalline plasticity formulation was used in a nonlinear finite element (FE) framework to understand how different GB orientations and GB-dislocation-density interactions affect local and overall behavior. An effective Burger's vector of residual dislocations was obtained for fcc bicrystals and compared with molecular dynamics (MDs) predictions of static GB energy, as well as dislocation-density transmission at GB interfaces. Dislocation-density pile-ups and accumulations of residual dislocations at GBs and triple junctions (TJs) were analyzed for a polycrystalline copper aggregate with Σ1, Σ3, Σ7, Σ13, and Σ21 CSLs and random high-angle GBs to understand and predict the effects of GB misorientation on pile-up formation and evolution. The predictions indicate that dislocation-density pile-ups occur at GBs with significantly misoriented slip systems and large residual Burger's vectors, such as Σ7, Σ13, and Σ21 CSLs and random high-angle GBs, and this resulted in heterogeneous inelastic deformations across the GB and local stress accumulations. GBs with low misorientations of slip systems had high transmission, no dislocation-density pile-ups, and lower stresses than the high-angle GBs. This investigation provides a fundamental understanding of how different representative GB orientations affect GB behavior, slip transmission, and dislocation-density pile-ups at a relevant microstructural scale.