A comparison between the experimental process parameters employed for the pulse plating of nanocrystalline nickel and the solution-side mass transfer and electrokinetic characteristics has been carried out. It was found that the experimental process parameters (on-time, off-time and cathodic pulse current density) for cathodic rectangular pulses are consistent and within the physical constraints (limiting pulse current density, transition time, capacitance effects and integrity of the waveform) predicted from theory with the adopted postulates. This theoretical analysis also provides a means of predicting the behaviour of the process subject to a change in the system, kinetic and process parameters. The product constraints (current distribution, nucleation rate and grain size), defined as the experimental conditions under which nanocrystalline grains are produced, were inferred from electrocrystallization theory. High negative overpotential, high adion population and low adion surface mobility are prerequisites for massive nucleation rates and reduced grain growth; conditions ideal for nanograin production. Pulse plating can satisfy the former two requirements but published calculations show that surface mobility is not rate-limiting under high negative overpotentials for nickel. Inhibitors are required to reduce surface mobility and this is consistent with experimental findings. Sensitivity analysis on the conditions which reduce the total overpotential (thereby providing more energy for the formation of new nucleation sites) are also carried out. The following lists the effect on the overpotential in decreasing order : cathodic duty cycle, charge transfer coefficient, Nernst diffusion thickness, diffusion coefficient, kinetic parameter (gamma) and exchange current density.