Based on the synergistic effect of hybridisation-superhydrophobicity, a simple and facile spraying method was used to achieve efficient sealing of Fe-based amorphous metallic coatings. In this paper, we employed rare-earth neodymium salts as inorganic sealant raw materials and loaded low surface energy fluorosilanes into epoxy resins to act as organic sealant raw materials. The surface structure and chemical composition of the sealing coatings were systematically characterised. The sealing mechanism as well as the anti-corrosion mechanism of the coating were investigated intensively. The results indicate that the superior corrosion resistance and self-cleaning ability of the sealed coating stems from the inorganic–organic-complex trinity effect: the corrosion inhibition effect of Nd oxide deposited during the inorganic sealing process, the shielding effect of the resin in the organic sealing, and the cross-linking and superhydrophobicity behaviour (liquid repellency effect) of the FDTES-Nd3+-Fe2+ complexes formed on the surface of the coating. This work provides valuable guidelines and insights for the design of subsequent corrosion-resistant and sealing coating.