The present paper introduces an intelligent anticorrosion coating, based on the mechanized hollow mesoporous silica nanoparticles (HMSs) as smart nanocontainers implanted into the self-assembled nanophase particles (SNAP) coating. As the key component, smart nanocontainers assembled by installing supramolecular nanovalves in the form of the bistable pseudorotaxanes on the external surface of HMSs realize pH-responsive controlled release for corrosion inhibitor, caffeine molecules. The smart nanocontainers encapsulate caffeine molecules at neutral pH, and release the molecules either under acidic or alkaline conditions, which make them spontaneously experience the pH excursions arisen from corrosion process and respond quickly. The intelligent anticorrosion coating was deposited on the surface of aluminum alloy AA2024 and investigated by electrochemical impedance spectroscopy and scanning vibrating electrode technique (SVET). Compared with the pure SNAP coating, the well-dispersed smart nanocontainers not only delay the penetration rate of corrosive species but also repair damaged aluminum oxide layer to maintain the long term anticorrosion behavior. From the experimental results of SVET, the smart nanocontainers with the acid and alkaline dual stimuli-responsive characteristics can simultaneously suppress corrosion activities on microanodic and microcathodic regions, demonstrating an excellent self-healing functionality.