The folk proverb “the older, the better” is usually used to describe the quality of Citrus grandis “Tomentosa” (CGT) in China. In this study, CGT aged for 6‐, 12‐, 16‐, and 19‐years were collected for the investigation of infusion color, main bioactive components, antioxidant activity, metabolic composition, and pathway. The results found that infusion color, the total phenolic and flavonoid, and antioxidant activity of CGT were obviously changed by aging process. Through untargeted metabolomics, 55 critical metabolites were identified to in discrimination of CGT with different storage ages, mainly including phenylpropanoids, lipids, and organic oxygen compounds. Twenty compounds that showed good linear relationships with storage ages could be used for year prediction of CGT. Kyoto encyclopedia of genes and genomes enrichment pathway analysis uncovered important metabolic pathways related to the accumulation of naringin, kaempferol, and choline as well as the degradation of benzenoids, thus supporting that aged CGT might be more beneficial to health. Correlation analysis provided that some key metabolites with bitter taste and biological activity were involved in the darkening and reddening of CGT infusion during aging, and total phenolic and flavonoid were more strongly associated with the antioxidant activity of CGT. This study systematically revealed the quality changes and key metabolic pathways during CGT aging at first time.Practical ApplicationThis study reveals the differences in quality attributes and metabolic profile between CGT with different storage ages, providing guidance for consumers' consumption, and also providing more scientific basis for the quality evaluation and improvement of CGT.