When zeolite catalysts are subjected to steam at high temperatures, a permanent loss of activity happens, because of the loss of aluminum from the framework. This dealumination is a complex process involving the hydrolysis of four Al–O bonds. This work addresses the dealumination from a theoretical point of view, modeling the kinetics in zeolite H-SSZ-13 to gain insights that can extend to other zeolites. We employ periodic density functional theory (DFT) to obtain free-energy profiles, and we solve a microkinetic model to derive the rates of dealumination. We argue that such modeling should consider water that has been physisorbed in the zeolite as the reference state and propose a scheme for deriving the free energy of this state. The results strongly suggest that the first of the four hydrolysis steps is insignificant for the kinetics of zeolite dealumination. Furthermore, the results indicate that, in H-SSZ-13, it is sufficient to include only the fourth hydrolysis step when estimating the rate of dealumination at temperatures above 700 K. These are key aspects to investigate in further work on the process, particularly when comparing different zeolite frameworks.