Owing to the advantages of organic field-effect transistors (OFETs) in the versatility of organic synthesis, multiparameter measurement, and signal amplification, sensors based on OFETs have received increasing attention for detecting volatile organic compounds (VOCs). However, false device operation and gas-sensing measurements often occur to vitiate the advantages of OFETs and even output error gas-sensing signals. In this work, by experimentally and theoretically studying the effects of VOC adsorption on the operational characteristics of the OFET, the proper operations of OFETs in gas-sensing measurements were clarified. The multiparameter measurements of OFETs showed that the source-drain current was the optimized parameter for achieving high responsivity, and other OFET parameters could be used for fingerprint analysis. By operating OFETs in the near-threshold region, the amplification effect was switched to enhance the responsivity by orders of magnitude to VOCs, while in the overthreshold region, the OFETs had a low signal-to-noise ratio. Besides, a counteraction effect and an uncertainty effect were discovered, leading to error gas-sensing signals. A theoretical study was carried out to reveal the dependency of the gas-sensing properties of OFETs on VOC adsorption. A series of rules were proposed for guiding the measurements of OFET sensors by taking full advantage of transistors in gas-sensing applications.