In this study, a novel nanostructure based on graphene nanosheets modified with inorganic/organic hybrid inhibitor based on zinc cations/walnut green shell extract (GO-Zn-WGSE) was synthesized and its corrosion protection properties were investigated in a silane-based matrix. The morphology and chemical composition of the synthesized GO-Zn-WGSE were investigated using field-emission scanning electron microscopy (FE-SEM) coupled with energy dispersive X-ray analysis (EDX), and Fourier transform infrared spectroscopy (FTIR). Interactions of components between graphene nanosheets, Zn2+ cations, and walnut green shell extract were assessed by thermogravimetric analysis (TGA), and ultraviolet–visible (UV-visible) spectroscopy. Corrosion inhibitive performance of GO-Zn- WGSE incorporated in the silane-based coating was studied using potentiodynamic polarization and electrochemical impedance spectroscopy (EIS). TGA and UV-visible results revealed the proper chelation between graphene nanoheets and inorganic and organic sections of modified GO-Zn- WGSE nanostructures. Also, inorganic/organic hybrid inhibitor showed a mixed-type inhibition mechanism with an efficiency of <90 %. Electrochemical measurements results showed that the addition of 0.2 wt. % G-Zn-FALE increased remarkably the self-healing corrosion protection performance of silane-based coatings.