Al alloy is widely used due to their excellent properties, but their poor corrosion and wear resistance limit broader applications. This study presents a novel two-step hydrothermal method to fabricate a superhydrophobic NiCo-LDH/MOFs@OPA composite film with long-term corrosion resistance, wear resistance, and self-cleaning properties. NiCoAl-LDH was first grown on anodized aluminum, followed by the formation of NiCo-MOFs using 2-methylimidazole (2-MI), and finally modified with octadecylphosphonic acid (OPA). The surface morphology, interfacial characteristics, corrosion resistance, and tribological performance of the composite film were systematically investigated. Characterization showed that MOFs effectively sealed LDH defects, greatly improving durability. After 28 days of immersion, the corrosion current density of NiCo-LDH/MOFs decreased to 4.846 × 10 −8 A·cm −2, two orders of magnitude lower than that of NiCoAl-LDH, and the NiCo-LDH/MOFs@OPA exhibited a corrosion current density as low as 7.627 × 10 −10 A·cm −2 and |Z| 0.01Hz > 10 8 Ω·cm 2. The OPA-modified film showed a contact angle of 158.1° and a sliding angle of 3.6°. Tribological tests confirmed excellent wear resistance with a stable friction coefficient down to 0.25. DFT calculations further revealed the interaction mechanism between MOFs and LDH. This work provides a promising approach for multifunctional coatings on aluminum alloys for harsh environments.