<p>In this study, α-ZrP two-dimensional nanomaterials were first prepared by hydrothermal synthesis, and then Ni-α-ZrP composite coatings were successfully prepared by pulsed electrodeposition to investigate the effects of α-ZrP materials on the surface morphology, mechanical properties, and corrosion resistance of Ni-based coatings. The successful synthesis of the materials was confirmed by SEM, TEM, and XRD. Subsequent analysis utilized the techniques of SEM, mapping, XPS, and XRD to characterize the coatings. Finally, the mechanical properties and corrosion resistance of the coatings were investigated. The findings showed that the Ni-α-ZrP composite coatings exhibited enhanced mechanical properties and corrosion resistance in comparison to Ni coatings. The Ni-α-ZrP-0.25 coating demonstrated optimal performance when the α-ZrP content was set at 0.25 g/L, at which point the coating attained its maximum hardness, accompanied by a substantial decrease in the coefficient of friction. The optimal impedance stands at <i>R</i>_c = 42,510 Ω∙cm², which is 7.3 times higher than that of the pure Ni coating. These findings indicate that α-ZrP significantly improves the wear and corrosion resistance of Ni coatings. This work provides a new perspective on the preparation of Ni-based coatings enhanced by two-dimensional lamellar materials via pulsed electrodeposition.</p>