The work aims to prepare a new type of magnetic abrasive particles to solve the processing difficulty of zirconia ceramics. Diamond/iron magnetic abrasive particles were prepared by bonding method. The effect of different composition ratios on the abrasive properties in the preparation process was investigated. The surface morphology of magnetic abrasive particles was analyzed by scanning electron microscopy (SEM). Combined with the grinding test of zirconia ceramics plate, the surface quality of the workpiece before and after grinding was compared and analyzed by surface roughness measuring instrument and 3D ultra-depth-of-field microscope to evaluate the grinding performance of magnetic abrasive particles and finally determine the better preparation process parameters of magnetic abrasive particles. When the pressing force was 0.3 MPa, the mass ratio of mixture to binder was 10∶1, and the mass ratio of 6101 epoxy resin, organosilicon resin and 651 curing agent was 4∶1∶5, the cutting edge number of magnetic abrasive particles, and the bonding strength and high-temperature resistance of binder reached the optimum technological parameters. After 40 minutes of grinding with the magnetic abrasive particles, the surface roughness (Ra) of zirconia ceramics plate was reduced from 1.493 μm to 0.116 μm. The original surface defects and process texture were removed effectively, and the surface quality was improved. Adding organosilicon resin in binder can solve the problem of insufficient holding force of the abrasive phase on the iron matrix. The Diamond/Iron magnetic abrasive particles prepared by this bonding method can process super hard zirconia ceramics materials successfully and can be used as good grinding medium in grinding, and meet the requirements of magnetic abrasive finishing.