Abstract: Enshi Yulu is one variety of the most distinctive steamed green tea native to Enshi Prefecture, due to its vibrant green color, fresh aroma, and smooth taste. However, a significant challenge can remain to balance between reduced bitterness and preserved green features during production. In this study, a systematic investigation was conducted to determine the variation in the bitterness and astringency of Enshi Yulu under varying withering. A combination of orthogonal experimental design and high-performance liquid chromatography (HPLC) was employed to determine the contents of catechins and caffeine in fresh tea leaves. Furthermore, the Response Surface method (RSM) was applied to optimize the withering parameters. The relationships among flavor factors were then visualized using a chord diagram. The results indicated that the content of catechin varied significantly under different withering conditions (P = 0.0020), while the content of caffeine shared no statistically significant changes (P = 0.1713). The optimal parameters of withering were identified as an initial moisture content of 77.07%, a withering temperature of 25.49°C, relative humidity of 60.24%, and wind velocity of 0.54 m/s. The ratio of non-ester catechins to ester catechins (NETCAT/ETCAT) reached 0.5041 under the optimal conditions. The bitterness of the tea soup was effectively reduced for a smoother profile and more refined flavor. This ratio also emerged as the critical indicator of flavor harmony, providing the quantitative attribute of optimal taste. The interrelationships among flavor factors were also visualized using a chord diagram. There were strong correlations between NETCAT/ETCAT and specific catechins. Among them, the most pronounced correlations were observed with the EGCG (epigallocatechin gallate, R² = -0.990) and ECG (epicatechin gallate, R² = -0.918), followed by EGC (epigallocatechin, R² = 0.753). Therefore, the catechin composition contributed the most influence on the sensory properties of Enshi Yulu tea. A well-balanced catechin profile was used to mitigate the bitterness with the green and fresh tea. The withering conditions were utilized to modulate the chemical composition of tea leaves and their subsequent impact on the sensory quality. Advanced analytical techniques (such as HPLC and RSM) were then combined with the data visualization. Traditional tea processing was also bridged with modern scientific approaches. The quality and the market competitiveness of Enshi Yulu tea were improved after optimization. Additionally, future studies can be focused on the interactions between catechins and the rest of flavor-related compounds, such as amino acids and volatile aroma substances, in order to gain a more holistic understanding of flavor formation. Advanced sensing technologies can also be incorporated for real-time monitoring of temperature, humidity, and chemical composition during withering, in order to enhance precision and reproducibility. Moreover, the artificial intelligence and machine learning algorithms in data analysis can be expected to further refine the optimization during tea production. In conclusion, the chemical dynamics during withering in Enshi Yulu tea can provide a robust framework to integrate modern technology with traditional techniques during tea production. The bitterness can be reduced to preserve green features during tea processing. Both quality and consumer satisfaction can be enhanced for the sustainable promotion of Enshi Yulu tea.