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Nanoencapsulation of α-tocopherol (α-TOC) by blending sodium oleate (NaOl) and rebaudioside A (RebA) was successfully prepared by self-assembly method under mild conditions. The optimized nanoemulsion showed the loading capacity of α-TOC was 30 wt% of sodium oleate. FTIR analysis suggested that hydrogen bonds and hydrophobic interactions were the major forces in α-TOC-NaOl/RebA complexes that were spherical and possessed well-distinguishable core-shell structures. The freeze-dried α-TOC-NaOl/RebA complexes had great stability under ambient conditions. The release profile of α-TOC showed a first-order kinetics reaching around 67.9% after 90 h at 25 °C. Nanoencapsulation improved dispersibility and greatly increased the antioxidant activity of α-TOC. Therefore, the stable α-TOC-NaOl/RebA core-shell complexes prepared from “generally recognized as safe„ (GRAS) ingredients have great potential to supplement α-TOC in food and cosmetic products.