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Intercropping with green manure is a soil-sustainable cultivation practice that has demonstrated positive impacts on tea growth and the soil environment in tea plantations. Nevertheless, research examining the effect of leguminous green manure varieties in tea plantations is scarce. This study aimed to analyze the tea quality and soil environment components in response to intercropping with three distinct leguminous green manures, Cassia sophera cv. Chafei 1 (CF), Sesbania cannabina (Retz.) Pers. (SC), and Chamaecrista rotundifolia (Pers.) Greene (CR), with 70% chemical fertilizer, and compare them to non-intercropped green manures with 100% chemical fertilizer (CK) in tea plantations. The findings indicated that intercropping with SC increased the amino acids content of tea leaves, the soil organic carbon (SOC), the soil acid phosphatase (ACP), the soil acid protease (ACPT), and the bacterial diversity compared to the CK treatment. Intercropping with CR improved the ACP activity and bacterial diversity while intercropping with CF improved the polyphenols. Proteobacteria, Acidobacteria, Actinomycetes, and Firmicutes were identified as the dominant bacterial taxa in tea plantations with intercropped green manure. A strong positive correlation was indicated between the SOC contents and the amino acids content in tea leaves after intercropping. A canonical correspondence analysis indicated significant associations between the ACP and the urease activity, and between the ACP and ACPT, and both were closely linked to SC. This finding provides an explanation that intercropping with SC may positively affect tea quality by influencing the SOC content, the soil enzyme activity, and the soil bacterial diversity. Green manure intercropping may replace part of chemical fertilizers, improve the soil environment in tea gardens, and enhance the quality of tea. These findings offer a theoretical reference for selecting leguminous green manure and advancing the sustainable development of tea plantations.