Wettability has a significant impact on the flow of oil during enhanced oil recovery (EOR) and profound effect on fluid distribution in oil fields. Mechanisms that influence the interaction between the injected water and the components of crude oil in the presence of carbonate rock samples were investigated. The main objectives of this study were to investigate the role of both rock mineralogy and the compositions of various oils as a function of asphaltene content on the destabilization of the aqueous film separating the oil from the substrate rock surface of carbonates using aqueous phases such as brine and carbonated water. The contact angles as a function of time were measured using brine and carbonated water and two types of crude oil on four types of rock samples. Once the exact contact angle has been determined, the compositions of various oils, based on asphaltene contents, were characterized to investigate the role of oil composition on the destabilization of the aqueous film separating the oil from the rock surface. Interfacial tensions (IFTs) of brine and two types of crude oil were also measured. Four types of rock samples from carbonate reservoirs, with different compositions, selected based on X-ray diffraction results were as follows: (1) 100% dolomite D(100), (2) 100% calcite C(100), (3) 67% dolomite + 33% calcite (D67 + C33), and (4) 37% dolomite + 63% calcite (D37 + C63). Two types of crude oil were used based on the asphaltene content obtained using the saturate, aromatic, resin, and asphaltene analysis. The contents of asphaltenes for crude-1 and crude-2 were 11.6 and 6.4 wt % and represented as (I-11.6) and (II-6.4), respectively. In this study, crude oil/brine/carbonate systems showed that (D37 + C63) gave the lowest contact angle value of 67 with 6.4 wt % of asphaltene content (II-6.4) and that D(100) gave the highest contact angle of 136 degrees with 11.6 wt % of asphaltene content (I-11.6). Brine was used as the external phase on both tests. On the other hand, using carbonated water as the external phase, the contact angle decreased from 97.6 degrees (D67 + C33) to 75.5 degrees (D37 + C63) for mixed dolomite/calcite systems. Decreasing the dolomite content in mixed dolomite/calcite systems caused a shift in contact angle from the oil negative intermediate wet to weakly water wet regardless of the saturating fluid phase. Also, using the adhesion tension approach, in defining surface wettability, shows that with the decrease in the contact angle values, adhesion tension shifted to positive directions with an increase in the degree of water wetness. This behavior was mainly due to the effect of type-II crude oil. The novelty of this study stems from studying the effect of rock mineralogy based on dolomite and calcite distribution and oil composition based on the asphaltene content in wettability alteration using aqueous phases such as brine and carbonated water. The results of both contact angle and IFT were implemented in adhesion tension using the Thomas Young equation as an alternative approach in defining surface wettability. This study will provide a better understanding of mineralogy/fluid/interaction, which is very crucial in the optimization of water injection and wettability reversal during the EOR process.