The microstructure and mechanical properties consisting of tensile behavior and hardness of bulk nanocrystalline Al-7.5Mg alloy were investigated. Grain refinement was achieved by cryomilling of atomized Al-7.5Mg powders, and then nanocrystalline powders blended with 15% and 30% coarse-grained Al-7.5Mg powders were consolidated by hot isostatic pressing (HIP) followed by extrusion to produce bulk nanocrystalline Al-7.5Mg alloys. Bimodal structures, which enhance ductility and toughness of nanocrystalline metals, were produced that consisted of nanocrystalline grains and elongated coarse-grain bands. Examination of indentation revealed unusual deformation mechanisms and interactions between the coarse-grain bands and nanocrystalline regions. The ductile coarse-grain bands underwent extensive plastic deformation near indentation, while nanocrystalline regions exhibited limited deformation.