A water-based high catalytic activity magnetorheological chemical finishing fluid (HCAMRCFF) was prepared and modified to enhance the chemical action strength in magnetorheological chemical finishing (MRCF) for single-crystal SiC. The fluid consisted of ferroferric oxide (Fe3O4) and chromium (Cr), deionized water (DW), polyethylene glycol (PEG) and oleic acid, and hydrogen peroxide (H2O2) as the composite catalyst particles, base carrier liquid, surfactants, and oxidant, respectively. HCAMRCFFs with different component concentrations were used to modify via evaluating their catalytic activity. Moreover, the MRCF experiments on SiC were conducted using the prepared HCAMRCFFs. The results show that the catalytic activity increases with an increase in the oxidant concentration. Furthermore, composite catalysts and composite surfactants can significantly improve their catalytic activity. The catalytic activity also increases with an increase in the concentration of composite catalysts. In the composite catalysts, increasing the Cr concentration can significantly enhance the catalytic performance. Composite surfactants can exert the relative superiority to enhance the catalytic activity. Compared with the unmodified finishing fluid, the catalytic activity of modified HCAMRCFF increases by 65.4%; the material removal rate (MRR) of SiC increases by 72.5% up to 635.621 nmh−1, and a surface with a roughness of 0.33 nm is obtained.