Changes in the crystalline structure of silk sericin and silk fibroin induced by gamma-irradiation in the atmosphere described. The crystalline structure of silk sericin which had been subjected to gamma-irradiation remained unchanged. However the decomposition temperature of the specimen decreased to about 230 deg C, when the total dose of ..gamma.. rays exceeded 4.6 Mrad. The structure of the silk 1 type crystal of silk fibroin in the solid state, with a low degree of molecular orientation, changed into the silk 2 type crystal, when the total dose of ..gamma.. rays exceeded 4.6 Mrad. No changes in the crystalline structure were observed in the solid state of the silk 2 type crystal regardless of gamma-irradiation. The decrease in the decomposition temperature of the specimen was attributed to the decrease in the molecular orientation. However, the molecular conformation of silk fibroin with a randomly coiled structure remained unchanged even after gamma-irradiation.