Alkaline-extracted walnut protein isolate (AWPI) shows poor solubility in aqueous solutions, resulting in relatively low emulsion capacity. This work investigated the influence of ellagic acid (EA) or epigallocatechin-3-gallate (EGCG) conjugation on the solubility and emulsifying properties of AWPI. The increase in polyphenol content and decrease in free amino and thiol groups of walnut proteins confirmed successful conjugation. AWPI polyphenol conjugates showed significantly reduced surface hydrophobicity, greatly enhanced surface charge, and consequently improved solubility. Circular dichroism (CD) results indicated that the polyphenol-conjugated AWPI contained relatively higher α-helical and lower β-sheet contents than AWPI. The antioxidant capacity of the polyphenol-conjugated AWPI was significantly enhanced. Additionally, polyphenol conjugation resulted in decreased mean particle sizes and increased surface charges of the walnut protein-covered oil droplets. The emulsions stabilized by AWPI-polyphenol conjugates were relatively more stable over a range of pH values (7.0–11.0) and thermal treatments (25°C–90°C). Moreover, they exhibited greater storage stability than those stabilized by unmodified AWPI.