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For industrial applications of III/V on Si heteroepitaxial structures on exactly oriented (001)Si substrates are a prerequisite. An approach for high-quality InP on (001)Si is the growth on a patterned substrate. We employed nanometer-scale patterning of Si substrates and discuss the results in the present paper. We used self-assembled nanometer-scale three-dimensional InP islands as a mask for further Si substrate patterning. InP islands were grown by metal-organic vapor-phase epitaxy at 400 °C and in some cases afterward transformed during annealing at 640 °C. The samples were etched at different temperatures and durations in KOH- and NaOH-based etchants. We also used maskless nanometer-scale patterning of the substrates by applying boiling water or steps of cleaning procedures. Atomic-force microscopy was used to determine the morphology of the samples and to evaluate the dimensions of the …