Strategies to improve tensile strength and ductility of pulsed electrodeposited nanocrystalline Co-Cu were investigated. Parameters of deposition, which are pulse current density, duty cycle, and pulse-on time were adjusted to produce nanocrystalline Co-Cu deposits with different microstructures and morphologies. The most significant improvement of strength and ductility was observed at nanocrystalline Co-Cu deposited, at a low duty cycle (10%) and a low pulse-on time (0.3 ms), with a high pulse current density (1000 A/m2). Enhancement of ductility of nanocrystalline Co-Cu was also obtained through annealing at 200 °C, while annealing at 300 °C leads to strengthening of materials with reduction of ductility. In the as deposited state, tensile strength and ductility of nanocrystalline Co-Cu is strongly influenced by several factors such as concentration of Cu, grain size, and processing flaws (e.g., crystal growth border, porosity, and internal stresses), which can be controlled by adjusting the parameters of deposition. In addition, the presence of various microstructural features (e.g., spinodal and phase decomposition), as well as recovery processes induced by annealing treatments, also have a significant contribution to the tensile strength and ductility.