This study addresses the low reactivity and poor toughness of diabase tailings (DT), a high-silica industrial byproduct, which restricts their large-scale application in geopolymer binders. To overcome these limitations, a dual-regulation strategy integrating stepwise low-temperature thermal activation (100, 200, and 300 °C) with standard curing (20 ± 2 °C, 95% RH) was developed. This approach aimed to enhance mineral dissolution kinetics and facilitate the formation of a dense, interconnected gel network. XRD, FTIR, and SEM analyses revealed significant decomposition of amphibole, pyroxene, and olivine, accompanied by increased release of reactive Si and Al species, leading to the formation of a compact N–A–S–H/C–A–S–H gel structure. Under optimized conditions (Si/Al = 2.6; activator modulus = 1.2), the geopolymer achieved a 7-day compressive strength of 42.3 ± 1.8 MPa, a flexural strength of 12.76 ± 1.6 MPa, and a flexural-to-compressive strength ratio of 0.308, demonstrating significant improvements in toughness compared with conventional binders. This green, energy-efficient strategy not only reduces energy consumption and CO₂ emissions but also provides a technically feasible pathway for the high-value reuse of silicate-rich mining wastes, contributing to the development of sustainable construction materials with enhanced mechanical performance.