Heterogeneous plastic deformation behavior of two bimodal ultrafine-grained nickel materials with different ultrafine-grained (UFG) and coarse-grained (CG) components fractions was investigated experimentally at the grain level. The prismatic specimens were deformed quasistatically up to 10% axial plastic strain using compression test at room temperature. The local microstructure of the initial and deformed samples was measured by electron backscattered diffraction pattern analysis in a scanning electron microscope. It was found that the plastic deformation of bimodal materials is highly heterogeneous and the degree of heterogeneity depends strongly on the grain size distribution and the volume fraction of the CG component. The large localized plastic strain within the coarse grains was observed during compression. The strain localization resulted in occurrence of debonding and cracks in the UFG region or in the interface between CG and UFG components.