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These results and conclusions were fully supported and augmented by molecular orbital calculations.Molecule-based field-effect transistors (FETs) are of great significance as they have a wide range of application prospects, such as logic operations, information storage and sensor monitoring. This account mainly introduces and reviews our recent work in molecular FETs. Specifically, through molecular and device design, we have systematically investigated the construction and performance of FETs from macroscale to nanoscale and even singl