Tea is one of the most popular beverages in the world. For the contribution to the taste and healthy functions of tea, amino acids and catechins are important components. Among different kinds of black teas in the world, Keemun black tea has the famous and specific fragrance, “Keemun aroma”. During the processing procedure of Keemun black tea, the contents of amino acids and catechins changed greatly, and the differences of these concentrations during processing varied significantly. However, a rapid and dynamic determination method during the processing procedure was not existed up to now. In order to find out a rapid determination method for the contents of amino acids and catechins during the processing procedure of Keemun black tea, the materials of fresh leaves, withered leaves, twisted leaves, fermented leaves, and crude tea (after drying) were selected to acquire their corresponding near infrared spectroscopy and obtain their contents of amino acids and catechins by chemical analysis method. The original spectra data were preprocessed by the Standard Normal Variate Transformation (SNVT) method. And the model of Near Infrared (NIR) spectroscopy with the contents of amino acids and catechins combined with Synergy Interval Partial Least squares (Si-PLS) was established in this study. The correlation coefficients and the cross validation root mean square error are treated as the efficient indexes for evaluating models. The results showed that the optimal prediction model of amino acids by Si-PLS contained 20 spectral intervals combined with 4 subintervals and 9 principal component factors. The correlation coefficient and the root mean square error of the calibration set were 0.955 8 and 1.768, respectively; the correlation coefficient and the root mean square error of the prediction set were 0.949 5 and 2.16, respectively. And the optimal prediction model of catechins by Si-PLS contained 20 spectral intervals combined with 3 subintervals and 10 principal component factors. The correlation coefficient and the root mean square error of the calibration set were 0.940 1 and 1.22, respectively; the correlation coefficient and the root mean square error of the prediction set were 0.938 5 and 1.17, respectively. The results showed that the established models had good accuracy which could provide a theoretical foundation for the online determination of tea chemical components during processing.