The In‐Sb bi‐layer (Si(111)‐2×2‐InSb surface reconstruction) was able to be prepared by 1 monolayer Sb adsorption onto Si(111)‐√7×√3‐In surface reconstruction, as well as results with 2×2‐In and √3×√3‐In. By using the √7×√3‐In surface reconstruction with higher In coverage, the area covered in the In‐Sb bi‐layer increased, and the area covered by 2×1‐Sb surface phase which caused by desorption of In atoms from In‐Sb bi‐layer decreased. The heteroepitaxial growth of InSb films on a Si(111)substrate via the In‐Sb bi‐layer was carried out by using two‐step growth procedure. The grown InSb films rotated by 30° with respect to Si substrate. Due to the decrease of the area covered by the 2×1‐Sb surface phase, the InSb crystals without rotation, which has poor crystal quality and electric properties, disappeared. Consequently, the electric properties of the films improved than those of the sample grown via 2×2‐In. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)