Localized electrodeposition (LED) was explored as an additive manufacturing technique with high control over process parameters and output geometry. The effect of variation of process parameters and changing boundary conditions during the deposition process on the output geometry was observed through simulation and experimentation. Trends were found between specific process parameters and output geometries in the simulations; trends varied between linear and nonlinear, and certain process parameters such as voltage and interelectrode gap were found to have a greater influence on the output than others. The simulations were able to predict the output width of deposition of experiments in an error of 8–30%. The information gained from this research allows for greater understanding of LED output, so that it can potentially be applied as an additive manufacturing technique of complex three-dimensional (3D) parts on the microscale.