Intercropping is one of the most widely used agroforestry techniques, reducing the harmful impacts of external inputs such as fertilizers. It also controls soil erosion, increases soil nutrients availability, and reduces weed growth. In this study, the intercropping of peanut (Arachishypogaea L.) was done with tea plants (Camellia oleifera), and it was compared with the mono-cropping of tea and peanut. Soil health and fertility were examined by analyzing the variability in soil enzymatic activity and soil nutrients availability at different soil depths (0–10 cm, 10–20 cm, 20–30 cm, and 30–40 cm). Results showed that the peanut–tea intercropping considerably impacted the soil organic carbon (SOC), soil nutrient availability, and soil enzymatic responses at different soil depths. The activity of protease, sucrase, and acid phosphatase was higher in intercropping, while the activity of urease and catalase was higher in peanut monoculture. In intercropping, total phosphorus (TP) was 14.2%, 34.2%, 77.7%, 61.9%; total potassium (TK) was 13.4%, 20%, 27.4%, 20%; available phosphorus (AP) was 52.9%, 26.56%, 61.1%; 146.15% and available potassium (AK) was 11.1%, 43.06%, 46.79% higher than the mono-cropping of tea in respective soil layers. Additionally, available nitrogen (AN) was 51.78%, 5.92%, and 15.32% lower in the 10–20 cm, 20–30 cm, and 30–40 cm layers of the intercropping system than in the mono-cropping system of peanut. Moreover, the soil enzymatic activity was significantly correlated with SOC and total nitrogen (TN) content across all soil depths and cropping systems. The depth and path analysis effect revealed that SOC directly affected sucrase, protease, urease, and catalase enzymes in an intercropping system. It was concluded that an increase in the soil enzymatic activity in the intercropping pattern improved the reaction rate at which organic matter decomposed and released nutrients into the soil environment. Enzyme activity in the decomposition process plays a vital role in forest soil morphology and function. For efficient land use in the cropping system, it is necessary to develop coherent agroforestry practices. The results in this study revealed that intercropping certainly enhance soil nutrients status and positively impacts soil conservation.