The performance of existing wind-operating triboelectric nanogenerators (TENGs) with various types is not sufficiently high for the operation of common electronic devices. Thus, these TENGs are currently used only for powering electronic devices with low power consumption such as sensors and light-emitting diodes (LEDs). Herein, high-performance double-contact friction wind-operating TENGs are obtained through the intercalation of an aluminum (Al) layer within a dielectric film. At a wind velocity of 15.1 m s-1, the TENG produces an open-circuit voltage (Voc) of 232 V and short-circuit current (Isc) of 0.256 mA at a frequency of 412 Hz. The maximum output power density is 32.8 W m-2 at an external load of 3 MΩ which can be used for powering 36 LEDs. The outstanding output power is originated from both the double-contact in a single oscillation and the intercalated Al layer, which contributes to the improved electrostatic induction at both dielectric sides. Double-contact friction wind-operating TENGs with the intercalated Al layer demonstrate the possibility of supplementary power sources that can be applied to electronic devices working in outdoor environments.