The effects of the thickness of the large-mismatched amorphous In 0.6 Ga 0.4 As buffer layer on In 0.3 Ga 0.7 As epi-films grown on a GaAs substrate have been systematically investigated. The In 0.3 Ga 0.7 As films with the In 0.6 Ga 0.4 As buffer layer of 0, 1, 2, and 4 nm thickness are grown by low-temperature molecular beam epitaxy (LT-MBE) and are characterized by X-ray diffraction (XRD) and transmission electron microscopy (TEM). It is found that the degree of relaxation and the crystallinity of the as-grown In 0.3 Ga 0.7 As films are strongly affected by the thickness of the amorphous In 0.6 Ga 0.4 As buffer layer. The thinner In 0.6 Ga 0.4 As buffer layer is not enough to efficiently release the misfit strain between the In 0.3 Ga 0.7 As epilayer and the GaAs substrate, while the thicker In 0.6 Ga 0.4 As buffer layer is unfavorable to trap the dislocations and prevent them from extending into the In 0.3 Ga 0.7 As epi-films. We have demonstrated that the amorphous In 0.6 Ga 0.4 As buffer layer with a thickness of 2 nm can advantageously prevent threading and misfit dislocations from propagating into the subsequent In 0.3 Ga 0.7 As epilayer and increase the degree of relaxation of the as-grown In 0.3 Ga 0.7 As, ultimately leading to a high-quality In 0.3 Ga 0.7 As film. Our novel buffer layer technology has triggered a simple but effective approach to grow high-crystallinity In 0.3 Ga 0.7 As epitaxial film and is favorable for fabrication of GaAs-based high-efficiency four-junction solar cells.