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Single-walled carbon nanotube (SWNT) arrays are the key to making integrated circuits smaller than 10 nanometers. Herein, a brand-new approach is proposed to efficiently prepare semiconducting (s-) SWNT arrays by implementing a simple phenylation to modulate the metallic SWNT bandgap through the radical reaction between SWNTs and benzoyl peroxide molecules. Electrical measurement indicates that the percentage of s-SWNTs in the functionalized arrays could be higher than 97.8% after phenylation, promoting its exceptional performance as a fi