Nanocrystalline Ni-Cu alloys with a Cu content of 6, 10, 19, and 32 wt.% were prepared by pulse electrodeposition. The microstructure and tensile properties of the nanocrystalline Ni-Cu alloys were characterized by x-ray diffraction, transmission electron microscopy, and tensile testing. The x-ray diffraction analysis indicates that the structure of the nanocrystalline Ni-Cu alloys is a face-centered cubic, single-phase solid solution with an average grain size of 18 to 24 nm, and that the average grain size decreased with increasing Cu content. The ultimate tensile strength (~1265 to 1640 MPa) and elongation to failure (~5.8 to 8.9%) of the Ni-Cu alloys increased with increasing Cu content. The increase in tensile strength results from the solid solution and fine-grain strengthening. Elemental Cu addition results in a decrease in stacking fault energy, an increase in work hardening rate, a delay in plasticity instability, and consequently, a higher plasticity.