As a condition for obtaining the silk I type crystal that has stability and high reproducibility, after dissolving silk fibroin crystalline part (Fcp), the changes of recrystallized crystal structure according to dialytic pH were examined by x-ray diffraction and differential thermal analysis. The Fcp was obtained from the aqueous solution of silk fibroin enzymatic proteolyzed by chymotrypsin. The crystal structure of Fcp showed silk II type. When the Fcp was dissolved by 10M LiBr aqueous solution, the Fcp1 showed the silk II type at pH 9. However, besides the silk II type, the silk I type structure begins to appear at pH 8 and only the silk I type structure was found below pH 6. On the other hand, the Fcp2 that calcium chloride was used in the dissolution found only the silk I type crystal structure below pH8.