Although tea (Camellia sinensis)/soybean (Glycine max) intercropping is widely applied in tea gardens, the underlying mechanisms driving tea quality promotion remain largely unclear. This study explores the effects of intercropping on tea quality, soil nutrient availability, and soybean growth and analyzes their mutual relationship. Field experiments revealed that intercropping increased tea leaf water extracts, polyphenols, and amino acids by 4.36–8.99%, 14.76–15.23%, and 14.73–16.36%, respectively, across two growth stages. Furthermore, intercropping boosted organic matter, available nitrogen (N), phosphorus (P), and potassium (K) in the tea rhizosphere. Enzyme activities, including acid phosphatase, alkaline phosphatase, urease, and β-glucosidase, were also elevated in tea/soybean intercropping. In soybean, shoot and root biomass, weight and number of nodules, and N, P, and K content increased over cultivation time. Correlation analysis showed that tea water extracts and polyphenols were positively linked to soil available P and alkaline phosphatase activities. Soybean root and nodule growth were correlated with soil N and P activation and tea water extracts, indicating that soybean-mediated underground interactions drive mineral nutrient mobilization in rhizosphere, further improving tea quality. This study provides mechanistic insights into tea/soybean intercropping, offering practical implications for sustainable tea cultivation practices.