AbstractIn this work, nanocontainers based on layered double hydroxide (LDH) loaded with two different corrosion inhibitors, namely 2-mercaptobenzothiazole (MBT) and cerium(III) nitrate, were prepared. MBT was intercalated into LDH galleries in anionic form by anion-exchange, while Ce3+ was fixed between polyelectrolyte layers on the surface of LDH-MBT nanoplatelets by the Layer-by-Layer (LbL) method. Both inhibitors were found in the modified LDHs (LDH-Mod) by X-ray diffraction and scanning electron microscopy coupled with energy dispersive spectroscopy. The release studies performed by UV-vis spectrophotometry indicated that the main triggering conditions for release of MBT from LDHs changed when LDH nanoplatelets were covered with polyelectrolytes. Furthermore, electrochemical impedance spectroscopy and DC polarization were used to investigate the effect in combining MBT− and Ce3+ within the same nanocontainer, for the corrosion protection of 2024-T3 aluminium alloy directly in solution as well as in a hybrid sol–gel coating. The obtained results open prospects for application of these systems as additives in multifunctional smart coatings.