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Synergetic self-healing anticorrosion behaviors, by forming a self-assembly protective layer and repairing coating passive barrier, exhibit great potential in handling the notorious metal corrosion phenomenon. Herein, we developed a nanofiber-supported anticorrosion coating with synergistic protection effects of both self-healing and active corrosion inhibition, via a facile electrospinning combined coating technique. Polycaprolactone (PCL) nanofiber integrated with 2-mecapobenzothiazole-loaded halloysite nanotubes (HNTs-MBT) is directly deposited on the surface of metal substrate, forming an interconnected fiber network framework. The encapsulated corrosion inhibitor MBT can be released by a pH-triggered manner to realize instant corrosion protections. Additionally, coating defects could be repeatedly repaired by continuous polymer fiber upon heat treatment and the anticorrosion efficiency effectively remained, even after three cycles of damage-healing. Moreover, the repaired coating also exhibited durable anticorrosion performance, mainly attributed to the synergetic effects of both thermal-triggered bulk healing and active corrosion inhibition. This type of dual-functional coating provides efficient anticorrosive performances and may show great promise in long-term corrosion protection.