During tea cultivation, diverse agroforestry is an important and established intercropping measure, with most studies concentrating on ecological service provision and economic returns. However, the response of soil nutrients and microbial community structures in long-term tea plantations with diverse agroforestry intercropping systems is poorly understood. In the present field study (2015), three intercropping agroforestry-tea patterns (Osmanthus-Tea (OT), Michelia-Tea (MT), Osmanthus-Michelia-Tea (OMT)) along with a study control (C) were examined in terms of these two knowledge gaps. Results showed that, in terms of tea cultivation, the OMT system is more suitable than the OT and MT systems. The OMT system significantly increased the total nitrogen (TN, 16.4%), total potassium (TK, 10.5%), available nitrogen (AN, 14.2%), available phosphorus (AP, 26.7%) and soil organic matter (SOM, 28.9%). The OMT system increased phylum Firmicutes and Bacteroidetes abundance by 35.8% and 9.6%. In addition, the OMT system enhanced the abundance of class Bacteroidia (99.5%), Erysipelotrichia (96.9%), Clostridia (93.5%) and Actinobacteria (19.6%), respectively. In general, the phylum bacteria Proteobacteria, Firmicutes, Actinobacteria accounted for the largest proportion of bacteria in all three intercropping systems. In this study, the abundance of Firmicutes, Actinobacteria, Proteobacteria, and Bacteroidetes were positively correlated with AN, SOM and TP. The results of the present study will help to develop a better understanding of the benefits imposed by different agroforestry intercropping systems on nutrient dynamics and microbial structural diversity during tea cultivation.