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Fractured moderate oil-wet carbonate reservoirs are the main productive formations in the Middle East. The change in wettability state toward water wetness beside interfacial tension (IFT) reduction is one of the potential scenarios for more oil recovery process. Smart water and natural surfactant injection into the porous media will alter the rock wettability and reduce IFT which consequently results in more oil sweep from untouched pores. In this paper, a novel natural surfactant (Alfalfa species) is introduced for EOR applications. IFT and contact angle tests were carried out between the oil phase, rock surface, Alfalfa natural surfactant, and surfactant—ion hybrid aqueous solutions. The results of Alfalfa natural surfactant showed a 29.29 mN/m reduction of IFT (63.39% IFT optimization) at the concentration of 4 wt% as the critical micelle concentration (CMC). Also, after addition of Alfalfa the wettability of rock tends to be more water-wet from the initial oil-wet state by application of Alfalfa because of 86.84° reduction of contact angle (49.91% wettability alteration). Solutions of calcium, magnesium, and sulfate ions were prepared as modified synthetic seawater at CMC of Alfalfa natural surfactant to investigate their synergistic influences on intensifying the optimizations of IFT and wettability alteration as hybrid solutions. IFT measurements of the hybrids demonstrated that among mentioned ions calcium brings the best results as it showed good synergistic effects with mentioned non-ionic natural surfactant in advancing the optimization of IFT reduction from 63.39 (surfactant solution) to 71.0 (surfactant—ion hybrid solution) percent. Also, contact angle measurements of the hybrids demonstrated that calcium ions gain the best results and advance the contact angle optimization from 49.91 (surfactant solution) to 61.8 (surfactant—ion hybrid solution) percent. Therefore, the solution of 3 times Ca concentrated seawater + CMC of surfactant selected to conduct imbibition tests as a displacement experiment based on the hybrid results and the candidate solution caused a 19.2% increase in oil recovery factor regarding seawater flooding and a total oil recovery factor of 62%. • Optimization of IFT and wettability conditions by application of Alfalfa species as a natural surfactant for chemical EOR • Enhancement of the mentioned optimizations by addition of smart ions to natural surfactant solutions • Synergistic effects of Alfalfa natural surfactant and Smart water • Improvement of oil recovery factor by introducing the optimum hybrid solution at reservoir temperature [ABSTRACT FROM AUTHOR]