The crystalline structure of a kind of nature yellow Silk, derived from the parents of hybrid between Bombyx mori and a yellow cocoon silkworm(natural resources of color cocoon) , and a wildly silkworm silk fibroin were studied by Ramam spectrum, X-ray diffraction spectrum and FT-IR spectrum. Results shown that: All kinds of the silk fibroins were crystal high polymer composing with the major conformation of β-fold (SilkII). The crystallization degree of Bombyx mori silk fibroin and the nature yellow silk fibroin were higher than the wildly silkworm silk fibroin, and the crystalline structure of the nature yellow silk fibroin was more close to Bombyx mori silk fibroin.