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Medical diagnosis technology based on convolutional neural networks (CNNs) has achieved good performance. In this study, we collected serum samples from 38 glioma patients and 45 healthy controls and used partial least squares (PLS) analysis to reduce the dimension of the data. Different levels of noise were added to the reduced data onto data augmentation, and the AlexNet, ResNet, and GoogLeNet fine‐tuning models were applied for classification. To evaluate the performance of the models, we used five‐fold cross‐validation. The accuracy rates of the AlexNet, ResNet, and GoogLeNet fine‐tuning models were 98.50%, 98.24%, and 99.50%, respectively. The model with the best classification effect was GoogLeNet. The specificity and sensitivity of this model were 98.98% and 98.48%, respectively. In addition, the area under the receiver operating characteristic (ROC) curve (AUC) of the established diagnostic model was 0.9949. The results showed that the combination of serum Raman spectroscopy and the PLS‐Gaussian‐GoogLeNet model achieved a good diagnostic effect for glioma. This method has high clinical application value and is worthy of further popularization. [ABSTRACT FROM AUTHOR]