A triboelectric nanogenerator (TENG) can effectively convert high entropy mechanical energy from the environment into electrical energy and has broad application potential in self-powered microelectronics and intelligent sensing fields. However, the low output performance of a TENG is one of the bottlenecks that restrict its commercial application. Herein, we design a high-performance and ultrastable wind-driven TENG using a zirconium carbide-zirconia core–shell nanoparticles/polyvinyl chloride (ZrC@ZrO2/PVC) composite membrane and polyamide (PA) membrane as matched triboelectric materials. The investigations indicate that doping 0.9 wt % ZrC@ZrO2 core–shell nanoparticles in the PVC matrix and using 1000-grit sandpaper as a template can effectively boost the surface charge density of the triboelectric layer, so that the output performance of TENG can be improved. The optimized TENG produces a peak output voltage of 367 V, a peak output current of 40 μA, and a maximum output power of 3.2 mW under a wind speed of 17.9 m/s, which can charge a 10,000 uF commercial capacitor from 0 to 3 V within 240 s. The stored energy can supply power for 27 light-emitting diodes (LEDs) connected in parallel. Moreover, the TENG maintains a stable output performance after continuous working for 16 h and a week. This study provides a simple approach to enhance the surface charge density of the friction layer by adding core–shell structured nanoparticles and constructing a rough surface structure.