The oxidation step in Oolong tea processing significantly influences its final flavor and aroma. In this study, a gas sensors detection system based on 13 metal oxide semiconductors with strong stability and sensitivity to the aroma during the Oolong tea oxidation production is proposed. The gas sensors detection system consists of a gas path, a signal acquisition module, and a signal processing module. The characteristic response signals of the sensor exhibit rapid release of volatile organic compounds (VOCs) such as aldehydes, alcohols, and olefins during oxidative production. Furthermore, principal component analysis (PCA) is used to extract the features of the collected signals. Then, three classical recognition models and two convolutional neural network (CNN) deep learning models were established, including linear discriminant analysis (LDA), k-nearest neighbors (KNN), back-propagation neural network (BP-ANN), LeNet5, and AlexNet. The results indicate that the BP-ANN model achieved optimal recognition performance with a 3−4−1 topology at pc = 3 with accuracy rates for the calibration and prediction of 94.16% and 94.11%, respectively. Therefore, the proposed gas sensors detection system can effectively differentiate between the distinct stages of the Oolong tea oxidation process. This work can improve the stability of Oolong tea products and facilitate the automation of the oxidation process. The detection system is capable of long-term online real-time monitoring of the processing process.