Mn0.8Fe2.2O4 magnetic nanocrystals (Mn0.8Fe2.2O4 MNCs) are synthesized by thermal treatment of a metal-organic framework (MOF) template, and their physicochemical properties are characterized in detail. The Mn0.8Fe2.2O4 MNCs exhibited highly efficient performance for the catalytic degradation of Bisphenol A (BPA) by peroxymonosulfate (PMS) activation at various initial pH, catalyst dosage, and PMS concentration. A leaching solution experiment evidenced that PMS activation by the Mn0.8Fe2.2O4 MNCs is a heterogeneous process. Interestingly, scavenging experiments and electron paramagnetic resonance (EPR) analysis demonstrated that HO center dot is the dominant radical for BPA degradation, rather than SO4 center dot-. The scavenger experiment indicated that the surface-bound radicals may play the crucial role for BPA degradation. Increasing Cl- or decreasing bicarbonate concentrations in solution enhanced the catalytic degradation process significantly through non-radical pathways. The Mn0.8Fe2.2O4 MNCs exhibited desirable stability and reusability, that the spent Mn0.8Fe2.2O4 MNCs could be significantly regenerated by thermal treatment at 450 degrees C in open air. Findings from this study would expand the applications of MOFs and also provide new insights into the enhancement of degradation efficiency during PMS activation processes.