A detailed investigation of the microstructure and mechanical properties has been conducted in pure nickel deformed to high strains using accumulative roll bonding (ARB). Samples have been investigated after different numbers of ARB cycles and the results have been compared with data for nickel processed by other deformation techniques, with particular focus on conventional rolling. It is found that the structural evolution in ARB-processed nickel is rapid at low strains followed by a slower evolution as the strain approaches ultrahigh levels. Comparing samples processed by ARB and conventional rolling to an identical nominal strain, the microstructure after ARB is more refined and contains a greater fraction of high angle boundaries. This enhanced refinement is attributed to the geometric accumulation of shear-strain influenced volumes as a result of the ARB process and large-draught rolling conditions. Based on the observations, it is suggested that the key strengthening mechanisms in deformed nickel are grain boundary and dislocation boundary strengthening, and that the strength-microstructure relationship can be expressed by a single parameter equation, σ-σ0 = k2dav-0.5, where k2 is a constant and dav is the average boundary spacing in the deformed microstructure. Abstract: A detailed investigation of the microstructure and mechanical properties has been conducted in pure nickel deformed to high strains using accumulative roll bonding (ARB).Samples have been investigated after different numbers of ARB cycles and the results have been compared with data for nickel processed by other deformation techniques, with particular focus on conventional rolling. It is found that the structural evolution in ARB-processed nickel is rapid at low strains followed by a slower evolution as the strain approaches ultrahigh levels.Comparing samples processed by ARB and conventional rolling to an identical nominal strain, the microstructure after ARB is more refined and contains a greater fraction of high angle boundaries. This enhanced refinement is attributed to the geometric accumulation of shear-strain influenced volumes as a result of the ARB process and large-draught rolling conditions. Based on *Manuscript Click here to view linked References 2 the observations, it is suggested that the key strengthening mechanisms in deformed nickel are grain boundary and dislocation boundary strengthening, and that the strength-microstructure relationship can be expressed by a single parameter equation, σ-σ 0 = k 2 d av -0.5 , where k 2 is a constant and d av is the average boundary spacing in the deformed microstructure.