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Carrier-free nanodelivery systems are fully self-assembled from active ingredients through interactions, offering the advantages of green, safe, and large-scale manufacturing. To improve the dispersion of Citrus × limon 'Rosso' peel essential oil (CEO) in water and boost the biological activity of CEO and tea polyphenols (TP), self-assembled CEO-TP colloidal dispersions (CEO-TP Colloids) were fabricated through sonication without surfactants or carriers. The optimal CEO and TP concentrations in the CEO-TP Colloids were determined to be 10.0 and 20.0 mg/mL by particle size and stability analyzer, respectively. The CEO self-assembled with TP to form spherical nanoparticles through hydrophobic and hydrogen-bonding interactions, whereas the CEO in CEO-TP Colloids weakened TP intramolecular aggregation. Meanwhile, the CEO-TP Colloids showed synergistic effects with better antibacterial, cellular antioxidant, and anti-inflammatory activities than single components. This study opens up the possibility of carrier-free co-delivery of hydrophobic and hydrophilic active components developed into food-grade formulations with multiple bioactivities., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Ltd. All rights reserved.)