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The process quality control of traditional Chinese medicine (TCM) is crucial for ensuring product quality and facilitating the internationalization. However, the quality control faces major challenges due to the complexity of chemical composition and influence of factors in the production process. With the aid of artificial intelligence and chemometrics, modern spectroscopic analysis techniques effectively extract chemical information from TCM and provide an intelligent guarantee for TCM analysis. This article reviewed the research progress of modern spectroscopic techniques combined with chemometrics methods in the process quality control of TCM over the past 20 years. The principles, advantages and disadvantages of the main spectroscopic techniques applied in TCM are firstly summarized. Then chemometric methods used in the analysis of TCM are introduced, including sample set grouping, preprocessing, variable selection, chemical pattern recognition and multivariate calibration methods. Finally, the applications of spectroscopic techniques with chemometrics in the process analysis of TCM are reviewed. These applications include geographical origin identification, adulteration determination, species identification and wild versus cultivated identification of herbal raw materials. They also cover component determination and monitoring, chemical analysis and biomarker assessment of herbal intermediates. Additionally, dissolution behavior analysis of preparations and identification of expired and unexpired samples of patent herbal products are discussed. Intelligent and digital analysis of the entire process will promote the modernization of TCM industry.