An investigation was conducted to examine the effect of molybdenum (Mo) content on the grain size, lattice defect structure and hardness of nickel (Ni) processed by severe plastic deformation (SPD). The SPD processing was applied to Ni samples with low (~0.3 at.%) and high (~5 at.%) Mo concentrations by a consecutive application of cryorolling and highpressure torsion (HPT). The grain size and the dislocation density were determined by scanning electron microscopy and X-ray line profile analysis, respectively. In addition, the hardness values in the centers, half-radius and peripheries of the HPT-processed disks was determined after ½, 5 and 20 turns. The results show the higher Mo content yields a dislocation density about two times larger and a grain size about 30% smaller. The smallest value of the grain size was ~125 nm and the highest measured dislocation density was ~60 × 10 14 m -2 for Ni-5% Mo. For the higher Mo concentration, the dislocation arrangement parameter was larger indicating a less clustered dislocation structure due to the hindering effect of Mo on the rearrangement of dislocations into low energy configurations. The resultsshow there is a good correlation between the dislocation density and the yield strength using the Taylor equation. The parameter in this equation is slightly lower for the higher Mo concentration in accordance with the less clustered dislocation structure.