The development of flexible wearable triboelectric nanogenerators (TENGs) has attracted great interest in the application of self-powered multifunctional electronic devices. However, the practical application of textile-based TENGs still faces numerous obstacles, such as low-output performance, high-cost, and complex structure. Herein, we reported a novel wearable TENG based on nickel–copper bimetallic hydroxide nanowrinkles (NC-TENG) to harvest the mechanical energy from human motion. The nickel–copper bimetallic hydroxide and polytetrafluoroethylene (PTFE) film form a triboelectric pair, which was grown on carbon cloth via a hydrothermal method. Owing to the nano-scale surface topography of nickel–copper bimetallic hydroxide nanowrinkles, the NC-TENG may achieve high-output performance. The maximum instantaneous V_oc and I_sc of NC-TENG (size: 1 cm × 1 cm) arrived at 328 V and 36.15 μA, respectively. Besides, the maximum output power density achieved was 1.323 mW cm⁻², which is 13 times the electrical output of the TENG based on the carbon cloth and PTFE film. This study demonstrates the promising potential of a novel TENG for wearable electronics.