The underlying structural origin of magnetic properties is still elusive in Fe-based amorphous alloys.In this study,distinctive soft magnetic properties were developed in Fe76Si9B1oPs amorphous ribbons through systematic design of annealing process.Combining with synchrotron radiation,high-resolution transmission electron microscopy and first principle ab initio molecular dynamic simulation,it is found that the atomic structural evolution both in short range order and medium range order is responsi-ble for the magnetic softness at proper annealing temperature.In short range,formation of separated and densely coordinated Fe-metalloid clusters is instigated to adapt energy minimization,resulting in strengthening of ferromagnetic exchange interaction locally.In medium range,a homogeneous exchange-coupling from the uniformly strong and weak ferromagnetic regions is generated,which significantly weakens magnetic heterogeneity and leads to the excellent magnetic softness.Our findings may provide an effective/promising pathway to modulate the magnetic properties for Fe-based amorphous alloys,and give a comprehensive and quantitative understanding of the structure-properties relationship in amor-phous materials.