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To use III‐V compound semiconductors as channel materials in the future advanced MISFETs with high performance, it is important to acheive the growth of III‐V‐on‐Insulator structures on Si substrates. As a first step to accomplish this, we propose the selective formation of InP only on localized areas of Si (100) substrate by molecular beam epitaxy (MBE). It was found that InP was selectively grown only on bare Si window areas, while not grown on native silicon oxide areas at elevated substrtate temperatures (500°C). It was also found that by decreasing the window size (0.7×0.7 μm2) only single grain of InP was grown on each bare Si window area. This indicates that the selective MBE growth of InP on Si substrate is possible. (© 2008 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim)