For the application of lightweight alloys, the corrosion and wear problems of magnesium-lithium (Mg-Li) alloys have always been important problems that cannot be ignored. The coupling protection of multiple technologies has gradually become a new trend. In this study, layered double hydroxides (LDH) nanosheet arrays were in-situ grown on Ni-P coating by the electroless plating technology combined with hydrothermal synthesis technology. The optimum deposition conditions (temperature-time-pH) were selected by orthogonal test. The surface morphology, structure, corrosion resistance and wear resistance of LDH/Ni composite coatings under different conditions were systematically studied by SEM, XRD, FT-IR, DSC, electrochemical and tribological tests. The growth mechanism of LDH suitable for Ni-P coating surface was proposed by analyzing the growth process of LDH nanosheet arrays. The results showed that the condition of 125 °C-12 h-13 was conducive to the growth of LDH nanosheet arrays. Compared with the Ni-P coating and the composite coating under other conditions, the LDH125°C-12h-13/Ni composite coating has the lowest self-etching current density (7.50 × 10−7 A·cm−2) and the average friction coefficient (0.35). The defect sealing effect and Cl− barrier property of LDH effectively improved the corrosion resistance of the coating. The frictional properties were improved by lubrication and heat absorption properties of LDH. In addition, it was found that the growth of LDH on the Ni-P coating surface followed the mechanism of “deposition nucleation-diffusion growth”.