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Previous research on manipulating microstructure for performance enhancement primarily focused on the surface of TENGs. In this study, an innovative bottom\u2013up strategic design to control the internal nano\u2010architecture for the enhanced output of TENG is proposed. This multiscale structural design strategy consists of defect chemistry (angstrom\u2010scale), surface modification (nano\u2010scale), and spatial regulation of nanoparticles (meso\u2010scale), which helps explore the optimal utilization of TENG's internal structure. After fine\u2010tuning the nano\u2010architecture, the output voltage is significantly increased. This optimized TENG serves as a robust platform for developing self\u2010powered systems, including self\u2010powered electrochemical chlorination systems for sterilization. Additionally, through the utilization of multiscale simulations (density functional theory, all\u2010atom molecular dynamics, and dissipative particle dynamics), the underlying mechanisms governing how the optimized nanoparticle\u2013polymer interface and spatial arrangement of nanoparticles influence the storage and transfer of charges are comprehensively elucidated. This study not only demonstrates the effectiveness of manipulating internal nano\u2010architecture to enhance TENG performance for practical applications but also provides invaluable insights into structural engineering for TENG advancement.<\/jats:p>","DOI":"10.1002\/smll.202400041","type":"journal-article","created":{"date-parts":[[2024,3,18]],"date-time":"2024-03-18T11:20:25Z","timestamp":1710760825000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":7,"title":["Enhancing the Output Performance of Triboelectric Nanogenerator Through Regulation of its Internal Nano\u2010Architecture"],"prefix":"10.1002","volume":"20","author":[{"given":"Jiawei","family":"Li","sequence":"first","affiliation":[{"name":"Key Laboratory of Marine Environmental Corrosion and Bio\u2010fouling Institute of Oceanology Chinese Academy of Sciences  Qingdao 266071 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