Acidification and heavy metal stress pose challenging threats to the terrestrial environment. This investigation endeavors to scrutinize the combined effects of vermicompost and steel slag, either singularly or in concert with Ryegrass (Lolium perenne L.), on the remediation of acidic soil resulting from sulfide copper mining. The findings illuminate substantial ameliorations in soil attributes. The application of these amendments precipitates an elevation in soil pH of 1.39–3.08, an augmentation in organic matter of 4.05–8.65, a concomitant reduction in total Cu content of 43.2–44.7%, and a marked mitigation in Cu bioavailability of 64.2–80.3%. The pronounced reduction in soil Cu bioavailability within the steel slag treatment group (L2) is noteworthy. Characterization analyses of vermicompost and steel slag further elucidate their propensity for sequestering Cu²⁺ ions in the soil matrix. Concerning botanical analysis, the vermicompost treatment group (L1) significantly enhances soil fertility, culminating in the accumulation of 208.35 mg kg⁻¹ of Cu in L. perenne stems and 1412.05 mg kg⁻¹ in the roots. Additionally, the introduction of vermicompost and steel slag enriches soil OTU (Operational Taxonomic Units) quantity, thereby augmenting soil bacterial community diversity. Particularly noteworthy is the substantial augmentation observed in OTU quantities for the vermicompost treatment group (L1) and the combined vermicompost with steel slag treatment group (L3), exhibiting increments of 126.04% and 119.53% in comparison to the control (CK). In summation, the application of vermicompost and steel slag efficaciously diminishes the bioavailability of Cu in the soil, augments Cu accumulation in L. perenne, induces shifts in the soil microbial community structure, and amplifies soil bacterial diversity. Crucially, the concomitant application of vermicompost and steel slag emerges as a holistic and promising strategy for the remediation of sulfide copper mining acidic soil.