Low-carbon stabilization/solidification (S/S) is of increasing importance as an option for the treatment of municipal solid waste incineration fly ash (MIFA). This study tailored four binders (e.g., ordinary Portland cement (OPC), calcium aluminate cement (CAC), phosphate-modified OPC, and phosphate-modified CAC) for S/S of MIFA and evaluated the cytotoxicity of treated MIFA by using A549 cell-based in-vitro assay. After S/S treatment, the leachability of Cr, Cu, Zn and Pb from MIFA decreased by 76.1%, 93.4%, 69.6%, and 85.5%, respectively. Spectroscopic analysis indicated that the hydration products determined the immobilization efficiencies of various binders, and strong bonding between metallic cations and phosphate enhanced the immobilization efficiency. The treated MIFA showed significantly lower cellular reactive oxygen species (ROS)-inducing abilities than original MIFA, in which with phosphate-modified OPC treated MIFA showed the lowest ROS levels. Intracellular ROS and multicytotoxicity results also revealed that the treated MIFA not only decreased the cytotoxicity-inducing capability but also enhanced the tolerant dosage of cytotoxicity, in which phosphate-modified S/S treatments showed more effective mitigation (25% less cytotoxicity) than plain cement treatments due to the high-efficiency immobilization of potentially toxic elements. This study develops a pioneering assessment protocol to measure the success of sustainable treatment of MIFA in human health perspective.