This work focuses on the simulation and control of a three-dimensional (3D) porous silicon thin-film deposition process that is used in the manufacture of thin-film solar cell systems. Initially, a solid-by-solid 3D kinetic Monte Carlo (kMC) model is introduced to simulate the porous silicon thin-film deposition process, and the simulation parameters are tuned to generate porous silicon films with porosity values that match available experimental data. A closed-form differential equation model then is introduced to predict the dynamics of the film porosity computed by the kMC model, and the parameters in this model are identified by appropriate fitting to open-loop kMC simulation results. Subsequently, a model predictive controller (MPC) is designed and implemented on the kMC model. Closed-loop simulation results demonstrate that the thin-film porosity can be regulated to desired values.