The role of Fe-6.5wt%Si as a soft magnetic material in motor and power generation will continue to increase as power and efficiency demands keep increasing due to high silicon steel’s superior magnetic and electrical properties when operated at high frequencies. However, the presence of brittle phases creates challenges for mass production of the materials and for machining the materials into parts with demanding geometries. Understanding the processing parameters controlling the presence of the brittle phases is necessary to promote high silicon steels as the superior soft magnetic material. This research pioneers the use of in-situ cooling rate thermal imaging analysis and a 2D Laue x-ray detector to quantify the relationship among processing parameters, final microstructure of melt-spun ribbons and the associated physical properties. These techniques reveal the superlattice peaks of the ordered B2/D03 phases separating them from the background A2 phase. Utilizing a variety of techniques investigating mechanical, electrical, and magnetic properties’ correlation to crystal structure alongside processing parameters a time temperature transformation curve can be generated