This work reports the performance of pseudoboehmite (PB)-silane hybrid coatings for the corrosion protection of AA2024-T3. A survey of the coating pretreatment and treatment steps was undertaken to reveal the electrochemical impact of such treatments on AA2024-T3 and its constituents, with testing also done on model microstructural analogs including Al–4Cu, Al2CuMg, and Al7Cu2Fe. The hybrid coating performs very well in immersion and salt-spray conditions. The protective effect of the PB pretreatment is not additive but synergistic. PB surface layers could be integrated as a precursor to subsequent coatings owing to the functionality they can impart to the surface.