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Tribopositive, scalable, and biocompatible materials are highly desired for high‐performance triboelectric nanogenerators (TENGs). In this study, polyethylenimine (PEI) functionalized N‐doped carbon dots (NCDs‐PEI) are synthesized and a novel approach to develop high‐output TENGs by incorporating high permittivity NCDs‐PEI into polyvinyl alcohol (PVA) as the tribopositive composite (CPP composite) is proposed for the first time. By systematically manipulating the mass ratio of NCDs/PVA and PEI‐functionalized concentration, the optimized CPP composite‐based TENGs (CPP‐TENGs) reveal a remarkable enhancement in power density by 28.5 times as compared with pure PVA‐based TENGs. The considerable electric outputs of CPP‐TENGs can be attributed to the synergistic effect of interfacial polarization enhanced permittivity of CPP composite and boosted surface charge density induced by dual charge transfer pathways. Moreover, CPP‐TENGs present superior high‐output stability, durability, and humidity‐resistance, and can also effectively drive electronics at different humidity and monitor human body movements. This work renders a simple, feasible, and scalable pathway to boost the electrical performance of TENGs for biomotion energy harvesting as well as providing insights for exploiting novel tribomaterials in the development of high‐output TENGs.

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