The electrochemical buffing (ECB) process primarily works on the principle of preferential dissolution by coupling of electrical, chemical, and mechanical actions. ECB is used to buff clean and hygienic nanoscale surface finish of high-purity components. Despite being well known, the process mechanism has not been discussed adequately in the literature, which makes process control and its use difficult. This work explores the various material removal mechanisms through numerical simulations to better understand and control the ECB process. The numerical results are found to match reasonably well with the experimental data. It is found from the simulation results that the flux of species generated is dominated by current density and interelectrode gap, whereas flow of electrolyte and rotation speed of buff-head primarily influence their migration. The simulation model also infers that convective flux contributes of order of 102 over to diffusion flux in species migration, whereas electrophoretic flux does not have a significant contribution.