The Fe 81.3 Si 4 B 13–x P x Cu 1.7 soft magnetic alloys with high Cu and proper P elements addition were synthesized with the aim of ensuring the amorphous forming ability (AFA) while expanding the crystallization window (CW). It is found that the atomic ratio of P/Cu of ∼3 is advantageous for AFA whereas a small amount of P addition promotes the precipitation of α-Fe grains and excessive P addition induces surface crystallization behavior of the present alloys. High Cu concentration can expand the annealing temperature ( T a ) window whereas proper P addition effectively expands the annealing time ( t a ) window. The Fe 81.3 Si 4 B 8 P 5 Cu 1.7 soft magnetic alloy was successfully synthesized with a large T a window of up to 130 °C and t a window of 90 min, which is a breakthrough for nanocrystalline alloys with high saturation magnetization. Microstructure analysis reveals that the ultra-wide CW is related to the unique nucleation mechanism, that is, the α-Fe grains are precipitated attaching to the Cu or CuP clusters and enveloping the Cu clusters, resulting in the high number density of α-Fe nanocrystals. The ultra-wide C-W promises the potential material in flexibly choosing the annealing process according to the performance.

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