Low salinity water injection (LSWI), an emerging Enhanced Oil Recovery (EOR) method, has proven to be effective in increasing oil recovery by wettability alteration. As low salinity water is injected into the reservoir, the pre-established equilibrium is disturbed. The chemical reactions among the oil/brine/rock system alters the existing wettability, resulting in enhanced oil recovery. Water-alternating-gas (WAG) injection is also a leading EOR flooding process in light to medium oil sandstone and carbonate reservoirs. A recently proposed hybrid EOR method, CO2 low salinity (LS) WAG injection, shows promise based on experimental and simulation studies, compared to LSWI or CO2 injection alone. Wettability alteration is considered as the dominant mechanism for CO2 LSWAG injection. In this study, a new displacement contact angle measurement which better mimics the actual displacement process taking place in a reservoir is used, aiming to investigate the effect of monovalent and divalent cations, CO2, and injection schemes. It is found that the injection of NaCl low salinity water alters the wettability towards slightly water-wet, and the injection of CaCl2 low salinity water alters the wettability towards slightly oil-wet. The injection of CO2 promotes water-wetness and geochemical reactions between oil and brine. Injection scheme of CO2 and NaCl low salinity water is more efficient than WAG cycle of CO2/NaCl in wettability alteration towards more water-wet. However, the opposite trend is observed with CaCl2 low salinity water, of which WAG cycle of CO2/CaCl2 is more efficient in altering wettability towards water-wet. The oil drop deformation process during LSWI resembles the process of oil removal using surfactant. As CO2 is introduced, due to the acidic effect of CO2 and ion exchange, it acts to wet the rock surface, leading to a more water-wet state. With introduction of CO2, the oil drop deformation resembles the “roll-up” oil removal process.