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To develop a novel asymmetric nanofiber membrane with antioxidant and antibacterial activities, biocompatible polyvinyl pyrrolidone (PVP) and polycaprolactone (PCL) were used as carriers to load water-soluble tea tree extract (TTE) and hydrophobic tea tree oil (TTO) via electrospinning and electrostatic spraying, respectively, which was named as TTE-PVP-3/TTO-PCL. The results show that uniform TTE-PVP nanofibers with an average diameter of 95 ± 27 nm could be obtained when the mass ratio of TTE to PVP was set as 1:3. Homogeneous TTO/PCL microspheres with an average size of 4.38 ± 0.79 µm could be obtained when the propulsion speed was 0.08 mm/min and the voltage was 10 KV. The activity study showed that TTE could only improve the antioxidant activity of TTE-PVP-3/TTO-PCL, while TTO could improve the antibacterial activity effectively. Under experimental conditions, the inhibition zones of TTE-PVP-3/TTO-PCL against Staphylococcus aureus and Escherichia coli were 7.50 ± 0.48 mm and 9.55 ± 0.45 mm, respectively, and its scavenging rates for 2,2-diphenylpicrylhydrazyl (DHPP) and hydroxyl radical were 59.79 ± 4.10% and 61.02 ± 4.95%, respectively. In conclusions, TTE-PVP-3/TTO PCL can be potentially used as a new kind of anti-oxidative and antibacterial wound dressings. [ABSTRACT FROM AUTHOR]