Organic surfactants have been utilized with different nanoparticles in enhanced oil recovery (EOR) operations due to the synergic mechanisms of nanofluid stabilization, wettability alteration, and oil-water interfacial tension reduction. However, investment and environmental issues are the main concerns to make the operation more practical. The present study introduces a natural and cost-effective surfactant named Azarboo for modifying the surface traits of silica nanoparticles for more efficient EOR. Surface-modified nanoparticles were synthesized by conjugating negatively charged Azarboo surfactant on positively charged amino-treated silica nanoparticles. The effect of the hybrid application of the natural surfactant and amine-modified silica nanoparticles was investigated by analysis of wettability alteration. Amine-surfactant-functionalized silica nanoparticles were found to be more effective than typical nanoparticles. Amott cell experiments showed maximum imbibition oil recovery after nine days of treatment with amine-surfactant-modified nanoparticles and fifteen days of treatment with amine-modified nanoparticles. This finding confirmed the superior potential of amine-surfactant-modified silica nanoparticles compared to amine-modified silica nanoparticles. Modeling showed that amine surfactant-treated SiO2 could change wettability from strongly oil-wet to almost strongly water-wet. In the case of amine-treated silica nanoparticles, a strongly water-wet condition was not achieved. Oil displacement experiments confirmed the better performance of amine-surfactant-treated SiO2 nanoparticles compared to amine-treated SiO2 by improving oil recovery by 15%. Overall, a synergistic effect between Azarboo surfactant and amine-modified silica nanoparticles led to wettability alteration and higher oil recovery.