Reliable energy modules and higher-sensitivity, higher-density, lower-powered sensing systems are constantly required to develop wearable electronics and the Internet of Things technology. As an emerging technology, triboelectric nanogenerators have been potentially guiding the landscape of sustainable power units and energy-efficient sensors. However, the existing triboelectric series is primarily populated by polymers and rubbers, limiting triboelectric sensing plasticity to some extent owing to their stiff surface electronic structures. To enrich the current triboelectric group, we explore the triboelectric properties of the topological insulator nanofilm by Kelvin probe force microscopy and reveal its relatively positive electrification charging performance. Both the larger surface potential difference and the conductive surface states of the nanofilms synergistically improve the charge transfer behavior between the selected triboelectric media, endowing the topological insulator-based triboelectric nanogenerator with considerable output performance. Besides serving as a wearable power source, the ultra-compact device array demonstrates innovative system-level sensing capabilities, including precise monitoring of dynamic objects and real-time signal control at the human-machine interface. This work fills the blank between topological quantum matters and triboelectric nanogenerators and, more importantly, exploits the significant potential of topological insulator nanofilms for self-powered flexible/wearable electronics and scalable sensing technologies.