The limited durability of conventional coatings in harsh environments demands innovative strategies to synergistically enhance corrosion resistance and mechanical robustness. The study focuses on the influence of the interlayer spacing of layered nanomaterials on the morphology, structure, and anti-corrosion and wear-resistant properties of coatings. Electrochemical tests revealed a tenfold reduction in corrosion current density (from 2.51 to 0.25 μA/cm 2) and a fivefold increase in impedance modulus (4.76 × 10 4 vs. 4.95 × 10 3 Ω·cm 2), surpassing conventional LDH-modified coatings. AFM nanoindentation demonstrated a 290 % improvement in elastic modulus (16.5 GPa vs. 4.2 GPa for baseline), indicating exceptional stiffness and deformation resistance. Meanwhile, tribological wear test data indicated that the wear resistance of the coating nearly doubled. The synergy leads to good long-term stability. This improvement enhances the passive corrosion protection capability of the composite coating system.