Magnetic abrasive finishing (MAF) is an efficient finishing process method using magnetic abrasive particles (MAPs) as finishing tools. In this study, two iron-based alumina magnetic abrasives with different particle size ranges were synthesized by the plasma molten metal powder and powder jetting method. Characterization of the magnetic abrasives in terms of microscopic morphology, phase composition, magnetic permeability, particle size distribution, and abrasive ability shows that the magnetic abrasives are spherical in shape, that the hard abrasives are combined in the surface layer of the iron matrix and remain sharp, and that the hard abrasives combined in the surface layer of the magnetic abrasives with smaller particle sizes are sparser than those of the magnetic abrasives with larger particle sizes. The magnetic abrasives are composed of α-Fe and Al2O3; the magnetic permeability of the magnetic abrasives having smaller particle sizes is slightly higher than that of the magnetic abrasives having larger particle sizes; the two magnetic abrasives are distributed in a range of different particle sizes; the magnetic abrasives have different magnetic permeabilities, which are higher than those of the larger ones; both magnetic abrasives are distributed in the range of smaller particle sizes; and AZ31B alloy can obtain smaller surface roughness of the workpiece after the grinding process of the magnetic abrasives with a small particle size.