Nanocomposites of hydroxyapatite-fibroin (HA-FB) were prepared using the biomimetic process. The Nanocomposites were detected with X-ray diffraction (XRD), thermogravimetric analysis (TGA), Fourier transform infrared spectroscopy (FTIR) and transmission electron microscopy (TEM). The FTIR results showed that chemical bond forms between HA nanocrystals and fibroin protein. The secondary structure of fibroin can be affected by the mineralization process. TGA results indicated the content of mineralized fibroin in the nanocomposites can be freely adjusted by changing the initial concentration of fibroin solution. TEM image showed that the diameter of the single mineralized nanofibrils is about 2-3 nm and the nanofibrils can aggregate into bundles with the size of 6-8 nm in width and 30-60 nm in length.