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The presence of bio-active compounds in Stachys byzantina (SB) extract has made it a powerful source of green inhibitors in controlling steel corrosion. In this study, it has been attempted to create a highly durable corrosion protective film on the surface of the metal with SB and divalent zinc (II) cations and investigated them by Electrochemical Impedance Spectroscopy (EIS) and Potentiodynamic polarization (PP) tests, and surface analysis methods. EIS results show that after 24 h of placing the steel samples in 3.5% NaCl solution containing 700 SB - 300 ZN, the synergistic corrosion inhibition behavior was about 92%. Besides, the results of the PP demonstrated a significant reduction of the i corr . Furthermore, surface analyses such as Field Emission Scanning Electron Microscopy/Energy Dispersive X-ray Spectroscopy (FE-SEM/EDS) and Atomic Force Microscopy (AFM) images illustrated the low metal surface degradation, which indicates that the mix of SB and Zn caused a protective layer creation on the surface, especially for SB 700 - Zn 300. Also, new compounds of graphitic materials' structure were made using SB extract which is a natural-based chemical, and investigated by Fourier-Transform Infrared Spectroscopy (FTIR) test, Grazing Incidence X-ray Diffraction (GIXRD) technique, Ultraviolet-visible spectroscopy (UV-Vis) analysis, and Raman spectroscopy., Competing Interests: Declaration of Competing Interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier B.V. All rights reserved.)