The prolonged duration of phytoremediation poses a risk of heavy metal dispersal to the surrounding environment. This study investigated a combined remediation approach for cadmium (Cd)- and arsenic (As)-contaminated soil by integrating phytoremediation with stabilization techniques. Bidens pilosa was utilized as the phytoremediator, and steel slag, pyrolusite, and FeSO4 were employed as stabilizing agents in the pot experiments. Key metrics such as soil moisture content, root length, plant height, and heavy metal concentrations in Bidens pilosa were measured to evaluate the remediation efficacy. Additionally, the bioavailability, leaching toxicity, and chemical forms of Cd and As, along with other soil properties, were analyzed. The results indicated that the optimal restoration effect was achieved by combining steel slag, pyrolusite, and FeSO4 with stabilizers in a ratio of 2:1:10. Additionally, the optimal dosage of these materials was found to be 9% by weight. Mechanistic studies, including heavy metal speciation analysis, X-ray photoelectron spectroscopy (XPS), and microbial community diversity analysis, revealed that the stabilization effects were primarily due to the interactions of anionic and cationic ions, chelation by organic acids secreted by plant roots, and enhanced microbial activity. A cost–benefit analysis demonstrated the technical, economic, and commercial viability of the combined remediation approach.