In this study, based on existing heavy oil extraction technology, combined with the mineral composition in a reservoir, the synergistic catalytic effect of reservoir minerals and exogenous catalysts under the reaction system of a hydrogen-rich environment not only reduces the viscosity of thick oil but also reduces the extraction cost and further improves the recovery rate of heavy oil. In this study, the impacts of different reservoir minerals and exogenous catalysts on the aquathermolysis of heavy oil were investigated. The research results showed that the sodium montmorillonite within the reservoir minerals exhibited an optimal catalytic effect, and the synergistic catalytic effect of sodium montmorillonite and catalyst C-Fe (catechol iron) resulted in a viscosity reduction rate of 60.47%. Furthermore, the efficiency of different alcohols as hydrogen donors was screened, among which ethanol had the best catalytic effect. Under the optimal reaction conditions, the viscosity reduction rate after the addition of ethanol was 75.25%. Infrared spectroscopy, elemental analysis, thermogravimetry, and differential scanning calorimetry were used to study the changes in heavy oil before and after hydrothermal cracking. Element analysis showed that the synergistic catalytic effect of sodium-based montmorillonite and catalyst C-Fe increased the hydrocarbon ratio from 0.116 to 0.117, and the content of S and N elements decreased. This fully confirms the catalytic effect of sodium-based montmorillonite and C-Fe catalyst for he hydrogenation reaction of the unsaturated carbon in heavy oil.