The aim of this work was to use bimodal microstructures to improve ductility and fatigue resistance of nanocrystalline (NC) and ultrafine-grained (UFG) materials while keeping the materials’ high strength. Nickel plates produced by pulsed electrodeposition were used as NC base material while as UFG base material high-purity nickel was processed by equal channel angular pressing. After different heat treatments, bimodal microstructures could be realized in the size ranges of NC/UFG and UFG/coarse grained (CG). While the UFG/CG nickel revealed an improved ductility but little influence on the fatigue resistance, the NC/UFG nickel shows an extraordinary fatigue resistance.