The thickness of the thin wetting film depends on disjoining pressure forces, and it evolves with pH evolution due to brine acidification at the physical and chemical conditions of geological carbon dioxide storage becoming thinner in response to dewetting. In the literature, molecular dynamic simulation (MDS) studies have been employed to understand the effect of pressure/capillary pressure on the thin wetting film evolution. In this paper, a theoretical approach based on the Frumkin–Derjaguin Equation (FDE), models of electric double layer repulsion, and van der Waals forces have been used for the calculation of the wetting film thickness. The approach excluded hydration forces contribution to disjoining pressure forces due partly to its poorly understood nature, and partly to the high salinity conditions encountered in geological carbon storage. Due to its promising global storage capacity compared to other lithologies, the carbon dioxide–brine–silica systems was chosen to simulate sandstone saline aquifers. The validation of the model benefited much from literature resources on data and a universal model of carbon dioxide–brine interfacial tension. Calculated results confirm pH-induced dewetting and they follow trends controlled by pH and pressure as found in the literature. The novelty of the paper can be seen from the fact that it has demonstrated a theoretical supplement to MDS studies in addition to justifying the fundamental utility and versatility of the FDE. Moreover, the paper links for the first time, a transcendental equation to the thin wetting film theory encountered in the carbon dioxide–solid–brine system found in geological carbon storage.