Trimethylamine (TMA), a representative volatile gas characterized by a strong, pungent odor, is widely recognized as an indicator for assessing fish freshness according to international standards. Despite its importance, the development of TMA sensors that offer high sensitivity, rapid response kinetics, selectivity, and operation at low temperatures remains a significant challenge. In this study, a highly sensitive In2S3/In2O3 gas‐sensing material with porous rod‐like structures for TMA detection was designed via an in situ sulfurization process. The sulfurization state of In2O3 was precisely controlled by adjusting the amount of thioacetamide. Gas sensing investigations reveal that sulfur incorporation markedly enhances sensor performance. The In2S3/In2O3 sensor, with an S/In molar ratio of 1/3, exhibited superior TMA sensing performance at 150°C, including the highest response (2.17 to 0.1 ppm and 8.17 to 10 ppm), rapid response/recovery times, excellent selectivity, and a low detection limit (0.05 ppm). Additionally, the sensor demonstrated good reproducibility and long‐term stability, highlighting its significant potential for applications in monitoring the freshness and quality of seafood.