Chè Shan Tuyet ( Camellia sinensis var. Shan) is one of the precious tea resources of Vietnam; however, there is little research on its chemical composition. The purpose of this study was to characterize the main quality components, such as free amino acids and catechins, in Camellia sinensis var. Shan and Camellia sinensis var. sinensis collected in the high mountain of Ta Xua, Son La, Vietnam by using an amino acid analyzer and liquid chromatography coupled with tandem mass spectrometry, respectively. Principal component analysis (PCA) discrimination analysis of chemical profiles revealed a clear metabolic difference between the young leaves of Shan Tuyet tea and mature leaves of the same variety and of sinensis tea. The amino acids serine, glutamic acid, arginine, ornithine, and aspartic acid contributed mainly to the discrimination and could be considered biomarkers for Shan Tuyet tea. The levels of caffeine and 7 catechins, catechin, catechin 3-gallate, epicatechin, epicatechin-3-gallate, epigallocatechin 3-gallate, gallocatechin, and gallocatechin 3-gallate, in young leaves of Shan Tuyet tea were significantly higher than in the other types. Notably, the pair correlation among catechins revealed strong coefficients of the epistructures and non-epistructures, which suggested that these compounds can be converted naturally to each other. The strong correlation between epicatechin-3-gallate and catechin 3-gallate with antiradical ABTS activity of Shan Tuyet tea leaves indicates that these 2 catechins are mainly responsible for the antioxidant activity. This is the first report on the bioactive compounds of Shan Tuyet tea, as well as its potential for the production of health supplements.