The present global energy shortage and climate crisis can be addressed by embracing recycling, reuse, and recovery; for example, this can be achieved by methodically utilizing the problematic wastes for energy harvesting. This research describes a novel approach for recovery and reutilization of waste material by incorporating dog fur waste into a triboelectric energy harvester; this was accomplished via a simple, inexpensive, and eco-friendly chemical processing to turn this problematic waste into a high-performance tribolayer. Due to the complications of operating practical devices with dog fur in its natural form, the dog fur waste was transformed for the first time into a uniform thin-film-based high-performance positive tribolayer. The optimization of the fabrication of the dog fur film featured hexagonal pyramid nanostructures, and a novel tribopair was selected and consisted of the dog fur-based film and a Teflon film; these films have very large differences in electron affinities. Based on this optimization and selection, we achieved an outstanding output voltage, current, and power density of 2021.46 V, 109.84 μA and 24,669.957 μWcm−2, respectively, along with appreciable mechanical stability during continuous operation up to 10,000 cycles. Our research demonstrates the potential for integration of green electronics and self-powered human-pet interaction systems while providing a sustainable approach to a circular bioeconomy.