Hazardous mine tailings (HMTs) dam failures can cause devastation to the ecology environment, people's lives and property, which require expensive and complicated remediation engineering systematacially. A cheap and sustainable inertization disposal is proposed for de-risking HMTs without any carbon emissions, stabilizing hazardous heavy metal cations within safety minerals and also sequestering CO2 in the process, simultaneously. Herein, lead-zinc tailings as target HMTs were inertized by using waste rice husk ashes (RHAs) and carbide slag (CS) with a certain ratio, and lead-zinc tailings hardened pastes (LZTHPs) were investigated based on the experimental performance, analytical characteristics, and simulation diffusion methods, to deeply unveil the minerals transformation mechanisms and long-term stability from the cation perspectives. Results revealed that LZTHPs’ compressive strength ranged from 1.04–4.73 MPa and leaching toxicity concentrations of Pb, Zn, Cr, and Cd reached 0.03 mg/L, 1.78 mg/L, 0.01 mg/L, and 0.01 mg/L, respectively. C-S-H gels (Type I and II), cation hydroxides and CO2 mineralization carbonates were the hydrates in LZTHPs. Pb (86%), Zn (78%), Cr (76%), and Cd (65%) were immobilized as residual state, and CO2 mineralization capacity was 0.16 kg/kg. The diffusion coefficient of Pb, Zn, Cr, and Cd below 4.48 × 10−10 cm2/s, 1.39 × 10−10 cm2/s, 4.72 × 10−10 cm2/s, and 0.30 × 10−12 cm2/s, which would be sufficient in most scenarios to adequately stabilize tailings. Diffusion control is the leaching mechanism of cations. After 100 years of simulation diffusion, the diffusion areas of Pb, Zn, Cr, and Cd are 1.33 × 10−3∼1.49 cm2, 2.47 × 10−4∼0.48 cm2, 2.47–8.61 × 10−4 cm2, and 1.49 cm2, respectively, and the environmental impact of LZTHPs was negligible. This study provides promising solutions for alleviating hazardous tailings dangerous, achieving sustainable development with zero-carbon emission, implying the concept of eliminating waste by waste, synchronously.