The harsh melt-spinning and annealing processes of high saturation magnetization nanocrystalline softmagnetic alloys are the biggest obstacles for their industrialization. Here, we proposed a novel strategy to enlarge the processing window by annealing the partially crystallized precursor ribbons via a heterostructured crystallization process. The heterostructured evolution of Fe84.75Si2B9P3C0.5Cu0.75 (at.%) alloy ribbons with different spinning rate were studied in detail, to demonstrate the gradient nucleation and grain refinement mechanisms. The nanocrystalline alloys made with industrially acceptable spinning rate of 25−30 m/s and normal annealing process exhibit excellent magnetic properties and fine nanostructure. The small quenched-in crystals/clusters in the free surface of the low spinning rate ribbons will not grow to coarse grains, because of the competitive grain growth and shielding effect of metalloid elements rich interlayer with a high stability. Avoiding the precipitation of quenched-in coarse grains in precursor ribbons is thus a new criterion for the composition and process design, which is more convenient than the former one with respect to the homogenous crystallization mechanism, and enable us to produce high performance nanocrystalline soft-magnetic alloys. This strategy is also suitable for improving the compositional adjustability, impurity tolerance, and enlarging the window of melt temperature, which is an important reference for the future development of composition and process.