Summer-autumn tea is characterized by high polyphenol content and low amino acid content, resulting in bitter and astringent teast. However, these qualities often lead to low economic benefits, ultimately resulting in a wastage of tea resources. The study focused on evaluating the effects of foliar spraying of glucosamine selenium (GLN-Se) on summer-autumn tea. This foliar fertilizer was applied to tea leaves to assess its impact on plant development, nutritional quality, elemental uptake, organoleptic quality, and antioxidant responses. The results revealed that GlcN-Se enhanced photosynthesis and yield by improving the antioxidant system. Additionally, the concentration of GlcN-Se positively correlated with the total and organic selenium contents in tea. The foliar application of GlcN-Se reduced toxic heavy metal content and increased the levels of macronutrients and micronutrients, which facilitated adaptation to environmental changes and abiotic stresses. Furthermore, GlcN-Se significantly improved both non-volatile and volatile components of tea leaves, resulting in a sweet aftertaste and nectar aroma in the tea soup. To conclude, the accurate and rational application of exogenous GlcN-Se can effectively enhance the selenium content and biochemical status of tea. This improvement leads to enhanced nutritional quality and sensory characteristics, making it highly significant for the tea industry.