Abstract: This study aimed to investigate the differences in volatile composition and aroma of different fractions of Osmanthus fragrans absolute purified by molecular distillation. Gas chromatography-mass spectrometry (GC-MS) combined with orthogonal partial least-squares discrimination analysis (OPLS-DA), P-value, variable importance in the projection (VIP), and relative odor activity value (ROAV) were used for analysis. The light, heavy, and residue fractions of Osmanthus fragrans absolute were analyzed. A total of 73 volatile components belonging to 8 major categories were detected in the three fractions, including 22 alcohols, 5 aldehydes, 10 acids, 3 phenols, 5 ketones, 17 esters, 5 alkanes, and 6 olefins. Alcohols were the main contributors to the volatile components in each fraction, and the types and relative contents of volatile components significantly differed among the fractions (P<0.05). The discrimination model achieved a classification accuracy of 98.2% for the volatile components of the three fractions. After analyzing and determining the 27 differential volatile components (VIP>1) of the three fractions, the key aroma contributing components (ROAV>1) of the 14 light fractions, 9 recombinant fractions, and 11 residue fractions were analyzed by the aroma profile analysis. Light fractions exhibited more intense floral, sweet, and pine woody aromas compared to recombinant and residue fractions. The light fractions had the highest types and relative contents of volatile components and showcased the most intense Osmanthus fragrans floral flavor. This study provided a theoretical basis for the comprehensive utilization of different fractions of Osmanthus fragrans absolute through molecular distillation using GC-MS combined with chemometrics methods.