A corrosion-resistant coating on an aluminum-containing substrate such as an aluminum substrate, an aluminum alloy substrate (e.g., AA 2024, AA 6061, or AA7075), or other aluminum-containing substrate includes a corrosion inhibitor-incorporated Zn—Al layered double hydroxide (LDH) layer and a sol-gel layer. A zinc salt and a corrosion inhibitor (e.g., a salt of an oxyanion of a transition metal such as a vanadate) is dissolved to form a zinc-corrosion inhibitor solution, and the substrate is immersed in or otherwise contacted with the solution to form the corrosion inhibitor-incorporated Zn—Al LDH layer on the substrate. A sol-gel composition is applied on the corrosion inhibitor-incorporated Zn—Al LDH layer of the substrate to form a sol-gel layer, and the sol-gel layer is cured.