Oil production faces challenges such as limited oil production from carbonate reservoirs, high oil production costs, and environmental issues. Chemical flooding as an enhanced oil recovery (EOR) method (CEOR) can increase oil production by the use of chemical additives such as surfactants into the reservoirs. Surfactants can increase oil recovery by interfacial tension (IFT) reduction and alteration of the rock wettability from oil-wet to water-wet. The synthesis of chemicals such as synthetic surfactants is usually costly and harmful to the environment. To solve these problems, many researchers have oriented on the use of natural surfactants instead of synthetic ones within the CEOR process. A new approach to increase the efficiency of CEOR is the synergizing of the chemical additives with nanoparticles as a hybrid fluid, which is known as the nanotechnology-assisted EOR method. In this research, a natural surfactant derived from Cyclamen persicum (CP) plant was extracted, and its performance was optimized with the zinc oxide/montmorillonite (ZnO/MMT) nanocomposite in a synergistic usage. At the optimum concentration of the surfactant, the measurements of the IFT and the contact angle show 57.78 and 61.58% optimizations, respectively. Also, in the presence of NaCl, the performance of CP is improved. IFT and contact angle measurements were also conducted for ZnO/MMT nanofluids and CP-ZnO/MMT as hybrid nanofluids. Results indicate that ZnO/MMT nanocomposites can alter the wettability of the carbonate rock to the water-wet state. Also, the CP-ZnO/MMT hybrid nanofluid shows a good potential in both IFT reduction and altering wettability from oil-wet to water-wet. Finally, to investigate the effects of solutions on increasing oil recovery factor (RF), the optimum concentrations of the surfactant, nanocomposite, and hybrid solutions were selected for dynamic core flooding experiments, and improvements showed oil RF increases of 8.2, 6, and 13%, respectively.