The magnetic abrasive powders have great influence on the magnetic abrasive finishing accuracy and efficiency. A new kind of Fe-based spherical magnetic abrasive particles with Fe2N precipitates and Fe4N matrix was successfully synthesized by gas nitriding. The results show that the prepared Fe-based magnetic abrasive particles can reduce the roughness of the Zirconium tube from 0.325 to 0.154 μm by four MAF passes. The high hardness and wear resistance of the Fe-based magnetic abrasive particles are assessed based on the Vickers hardness and nanoindentation results. This study can provide theoretical and experimental support for fabricating high-performance magnetic abrasive particles.