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Round green tea (RGT) is widely distributed and presents a high yield in China. The quality of RGT can be determined by its aroma; however, the transformation and formation of volatile metabolites during RGT processing remain unclear. In this study, 173 volatile compounds (nine categories) were identified totally from RGT via gas chromatography-mass spectrometry with infrared-assisted headspace-solid phase microextraction. These substances exhibited different changing trends during various procedures, with the most intense transformation occurring during fixation, followed by pan-frying and second drying; moreover, 51 substances were screened, mainly containing fatty acid-derived volatiles (i.e., (E)-2-hexen-1-ol, Hexanal, pentanal, hexanal) and glycoside-derived volatiles (i.e., linalool, geraniol, benzyl alcohol, benzaldehyde), and their evolution during processing was clarified. Furthermore, the effect of the second-drying temperature on volatile compound metabolism was clarified, and 90°C was the best temperature for RGT aroma. This research lays a foundation for in-depth quality control and the aroma formation mechanism of RGT.