This study was to examine the formation of advanced glycation end-products (AGEs) in black tea during drying process at 90, 120, and 150 °C for 1 h. Nine AGEs including Nɛ-(carboxyethyl)-L-lysine (CEL), Nɛ-(carboxymethyl)-L-lysine (CML), three isomers of methylglyoxal-hydroimidazolones (MG-Hs), three isomers of glyoxal-hydroimidazolones (GO-Hs), and argpyrimidine were quantified by using HPLC-MS/MS with isotope-labelled internal standard. Results showed that each AGE during the drying process of 150 °C was significantly higher (p < 0.05) than at 90 and 120 °C, and argpyrimidine was only found in the treatment of 150 °C. MG-H1/3 was first quantified as the major AGE during drying at 120–150 °C, the content respectively reached to (39.66 ± 2.61) μg/g and (58.88 ± 1.76) μg/g after 1 h drying, where CML content only had (19.86 ± 1.02) μg/g and (23.71 ± 1.40) μg/g. This study indicated that arginine derived-AGEs are the key components of black tea AGEs.