Single-atom catalysts (SACs) are emerging as potent tools for the selective regulation of active species, offering substantial promise for green and sustainable Fenton catalysis. However, current SACs face limitations due to the specificity of their supports, which only allow selective regulation within certain oxidant systems. This constraint makes targeted regulation across different systems challenging. In response, this study designs a SAC, termed CoSAs-ZnO, featuring surface hydroxylation and an isolated asymmetric Co-O-Zn configuration. This SAC can realize a nearly 100% selective generation of sulfate radicals (SO