The overall dissolution of silicate minerals is controlled by multiple surface reaction mechanisms, reflecting the complex structure of the surface at both molecular- and micrometer-scale levels. This complexity results in a large number of possible local atomic configurations influencing site reactivity and thus a corresponding variability in surface reactivity. The aim of this study is to elucidate the net kinetic effect of multiple reactions taking place at the silicate–water interface using kinetic Monte Carlo (KMC) simulations. However, achieving the proper balance in the number of model parameters required to adequately describe a system’s evolution versus the size of the system can be difficult. We approach this problem through the development of a sequence of computer models that consider details influencing surface site reactivity. The capabilities of these models are tested by simulating the dissolution of (001), (100), and (101) quartz faces. Quartz is used as a representative mineral for silicate structures because of its simple chemical composition, the availability of ab initio calculations, and its widespread distribution in the Earth’s crust and surface. The results show how the ability of each model to correctly predict or reproduce experimentally observed dissolution behavior of the quartz surface depends on model complexity, initial surface structure, and model parametrization. The successful analysis of mechanistic relationships between input parameters and simulation results demonstrates the power of KMC methods in evaluating mineral dissolution kinetics and identifying critical dissolution controls.