The introduction of poly(tannic acid) (PTA) and cerium ion [Ce(III)] on the surface of α-zirconium phosphate (α-ZrP) endowed the α-ZrP@PTA-Ce(III)/waterborne epoxy composite coating with enhanced corrosion protection and wear resistance performances. The successful preparation of α-ZrP@PTA-Ce(III) was confirmed through X-ray diffraction, X-ray photoelectron spectroscopy, and Fourier transform infrared spectra. PTA improved the compatibility between α-ZrP@PTA-Ce(III) and the waterborne epoxy resin due to the presence of organic groups from tannic acid. The wear resistance test indicated that the incorporation of α-ZrP@PTA-Ce(III) effectively reduced the coefficient of friction and the wear rate. Electrochemical impedance spectroscopy was used to analyze the corrosion protection performance of unbroken coatings and the self-healing ability of scratched coatings. The incorporation of α-ZrP@PTA-Ce(III) improved the protection performace distinctly. In addition, α-ZrP@PTA-Ce(III) endowed the composite coating with dual corrosion inhibition effects, originating from the PTA film, to prevent the penetration of corrosive media and a dense film that came from the Ce(III) cation. The waterborne epoxy system with enhanced corrosion and wear resistance in this paper broadens the application of α-ZrP.