The influences of legume diversification on soil carbon (C) pools and sequestration, particularly in Himalayan pastureland, remain poorly understood. Moreover, the impact of legume diversification activities and the stoichiometry of soil enzymes in C biogeochemistry at the ecosystem level remains largely overlooked. The purpose of this study is to investigate the influences of legume diversification on activities and the stoichiometry of soil enzymes and their control of C sequestration in pasturelands. Four experimental fertilized species combinations, namely, SG (50% Festuca arundinacea + 50% Dactylis glomerata), SGL1 (25% Festuca arundinacea + 25% Dactylis glomerata + 50% Onobrychis viciifolia), SGL2 (25% Festuca arundinacea + 25% Dactylis glomerata + 50% Trifolium pratense), SGL12 (25% Festuca arundinacea + 25% Dactylis glomerata + 25% Onobrychis viciifolia + 25% Trifolium pratense), and natural pasture (NG) were compared. Soils under SGL1, SGL2, and SG12 had ~18, 36, and 22% greater soil C than SG, respectively. Among the pastures with fertilization, the C mineralization was suppressed by legume diversification. C sequestration under SGL1, SGL2, and SG12 was ~27, 22, and 38% higher than SG, respectively, at the 0–30 cm soil layer. The ratios of DHA are as follows: for PhOX and DHA, PerOX significantly decreased with an increasing grass–legume mixture, suggesting greater C sequestration. PCA analysis revealed that C sequestration under legume diversification and enzymatic stoichiometry had an indirect but substantial impact on C sequestration. The increasing C sequestration under SGL12 was complemented by higher productivity. Data suggested that increasing legumes in pastureland might greatly enhance ecosystem functions such as soil C storage, productivity, ecorestoration efficiency, and biological activity in Indian Himalayan pastureland.