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In this study, we initially performed interfacial tension (IFT) tests to investigate the potential of using the Persian Gulf seawater (PGSW) as smart water with different concentrations of NaCl, KCl, MgCl2, CaCl2, and Na2SO4. Next, for each salt, at the concentration where IFT was minimum, we conducted contact angle, zeta potential, and micromodel flooding tests. The results showed that IFT is minimized if NaCl or KCl is removed from PGSW; thus, for solutions lacking NaCl and KCl, the IFT values were obtained at 26.29 and 26.56 mN/m, respectively. Conversely, in the case of divalent ions, minimum IFT occurred when the concentration of MgCl2, CaCl2, and Na2SO4 in PGSW increased. Specifically, a threefold rise in the concentration of Na2SO4 further reduced IFT as compared to optimal concentrations of MgCl2 or CaCl2. It should be mentioned that eliminating NaCl from PGSW resulted in the lowest IFT value compared to adding or removing other ions. Whereas the removal of NaCl caused the contact angle to decrease from 91.0° to 67.8° relative to PGSW and changed surface wettability to weakly water-wet, eliminating KCl did not considerably change the contact angle, such that it only led to a nine-degree reduction in this angle relative to PGSW and left wettability in the same neutral-wet condition. At optimal concentrations of MgCl2, CaCl2, and Na2SO4, only an increase in Na2SO4 concentration in PGSW could change wettability from neutral-wet to weakly water-wet. For solutions with optimal concentrations, the removal of NaCl or KCl caused the rock surface to have slightly higher negative charges, and increasing the concentration of divalent ions led to a small reduction in the negative charge of the surface. The results of micromodel flooding indicated that NaCl-free PGSW could raise oil recovery by 10.12% relative to PGSW. Furthermore, when the Na2SO4 concentration in PGSW was tripled, the oil recovery increased by 7.34% compared to PGSW. Accordingly, depending on the conditions, it is possible to use PGSW so as to enhance the efficiency of oil recovery by removing NaCl or by increasing the concentration of Na2SO4 three times.