| Summary: | The microstructure of the organic semiconductor (OSC) active layer is one of the crucial topics to improve the sensing performance of gas sensors. Herein, we introduce a simple solvent vapor annealing (SVA) process to control 6,13-bis(triisopropylsilylethynyl)-pentacene (TIPS-pentacene) OSC films morphology and thus yields high-sensitivity nitrogen organic thin-film transistor (OTFT)-based nitrogen dioxide (NO<sub>2</sub>) sensors. Compared to pristine devices, the toluene SVA-treated devices exhibit an order of magnitude responsivity enhancement to 10 ppm NO<sub>2</sub>, further with a limit of detection of 148 ppb. Systematic studies on the microstructure of the TIPS-pentacene films reveal the large density grain boundaries formed by the SVA process, improving the capability for the adsorption of gas molecules, thus causing high-sensitivity to NO<sub>2</sub>. This simple SVA processing strategy provides an effective and reliable access for realizing high-sensitivity OTFT NO<sub>2</sub> sensors.
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