In this study, an optimized yellowing process for yellow tea (YT) was developed by response surface methodology. The results showed that increasing the yellowing temperature from 20°C to 34°C, increasing the relative humidity from 55% to 67%, and reducing the yellowing time from 48h to 16h, caused a 40.5% and 43.2% increase in the yellowness and sweetness of YT, respectively, and improved the consumer acceptability by 36.8%. Moreover, metabolomics was used to explore the involved mechanisms that resulted in the improved YT quality. The optimized yellowing promoted the hydrolysis of 5 gallated catechins, 6 flavonoid glycosides, theogallin and digalloylglucose, resulting in the accumulation of 5 soluble sugars and gallic acid. Meanwhile, it promoted the oxidative polymerization of catechins (e.g., theaflagallin, δ-type dehydrodicatechin and theasinensin A), but decelerated the degradation of chlorophylls. Overall, this optimized yellowing process could serve as a guide to a shorter yellowing cycle.