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With increasingly severe metal corrosion, coating preparation with high-performance corrosion protection has attracted more attention. Herein, the encapsulation of the corrosion inhibitor 8-hydroxyquinoline (8-HQ) as well as the self-healing agent linseed oil (LO) in polyvinyl alcohol (PVA) and chitosan (CS) shells were realized by coaxial electrospinning, which was recorded as PVA/CS@LO/8-HQ core–shell nanofibers. PVA/CS@LO/8-HQ nanofibers were employed to promote the high-performance corrosion protection of the epoxy coating. The anticorrosion mechanism was that the change of the local pH on the metal surface stimulated the release of 8-HQ from the nanofibers, which were then chelated with iron ions to form a complex. When cracks occurred and caused rupture of the nanofibers, LO was released and reacted with oxygen to cure them so that the cracks could be healed autonomously. The dynamic potential polarization curves showed that the corrosion inhibition efficiency of the compound inhibitor LO + 8-HQ reached 87.54%, 90.31%, and 85.57% at pH = 3, 7, and 11, respectively, higher than that of the single corrosion inhibitor. Density functional theory calculations revealed that the LO and 8-HQ combination, forming a hydrogen bond interaction, promoted the adsorption of inhibitors on the steel surface. Scanning Kelvin probe and electrochemical impedance spectroscopy proved the self-healing corrosion protection properties of the epoxy coating. These results demonstrated that embedding PVA/CS@LO/8-HQ nanofibers in the coating could obtain self-healing properties, and promote the mechanical and corrosion protection of epoxy coating.