Although Enshi Yulu tea (ESYL) possesses a distinctive fragrance, there is a scarcity of studies focusing on its primary volatiles or aroma genesis. This study aims to elucidate the dynamics in the profiles of aromas and volatiles through aroma profiling analysis and headspace solid-phase microextraction/gas chromatography-mass spectrometry. A total of 10 aroma attributes and 128 volatiles were identified in ESYL, with geraniol and linalool exhibiting the highest levels, and alcohols constituting the predominant proportion. Besides, a relative odor activity value (ROAV) based molecular aroma wheel was constructed, revealing 12 key odorants with ROAVs >1, wherein linalool, β-ionone, and nonanal ranked highest. Notably, steaming and final drying emerged as critical steps for ESYL aroma development, while the non-enzymatic degradation of fatty acids likely contributed to the formation of its fresh aroma. These findings significantly enhance our comprehension of ESYL aroma formation.