Most fractured carbonate oil reservoirs have oil-wet rocks. Therefore, the process of imbibing water from the fractures into the matrix is usually poor or basically does not exist due to negative capillary pressure. To achieve appropriate ultimate oil recovery in these reservoirs, a water-based enhanced oil recovery method must be capable of altering the wettability of matrix blocks. Previous studies showed that carbonated water can alter wettability of carbonate oil-wet rocks toward less oil-wet or neutral wettability conditions, but the degree of modification is not high enough to allow water to imbibe spontaneously into the matrix blocks at an effective rate. In this study, we manipulated carbonated brine chemistry to enhance its wettability alteration features and hence to improve water imbibition rate and ultimate oil recovery upon spontaneous imbibition in dolomite rocks. First, the contact angle and interfacial tension (IFT) of brine/crude oil systems were measured for several synthetic brine samples with different compositions. Thereafter, two solutions with a significant difference in WAI (wettability alteration index) but approximately equal brine/oil IFT were chosen for spontaneous imbibition experiments. In the next step, spontaneous imbibition experiments at ambient and high pressures were conducted to evaluate the ability of carbonated smart water in enhancing the spontaneous imbibition rate and ultimate oil recovery in dolomite rocks. Experimental results showed that an appropriate adjustment of the imbibition brine (i.e., carbonated smart water) chemistry improves imbibition rate of carbonated water in oil-wet dolomite rocks as well as the ultimate oil recovery.