Silk fibroin is becoming a promising biomaterial because of its excellent biocompatibility. However, the regenerated fibroin is usually soluble in water and its mechanical properties should be improved. Although many methods, such as adding other polymers or treating with methanol, can ameliorate the mechanical properties and insolubility, the biocompatibility of fibroin is usually damaged in these processes. In this article, it is first reported that the insoluble fibroin films are directly prepared without methanol treatment. According to the results of Fourier transform infrared spectroscope (FTIR) and the X-ray diffraction (XRD), the amount of β-sheet conformation increased with the increasing of concentration. When fibroin films are dried from 15 wt% at 60℃, the films become insoluble in water. More importantly, The tensile strength and elongation of the insoluble fibroin films dried from 15% solution at 60℃ reached 15.9 MPa and 49.4% respectively in the wet state, which is distinctly superior to the fibroin films treated with methanol.