The material properties of III-V semiconductors are in many ways superior to those of Si. Examples of these properties are the possibilities for high electron mobilities and the direct bandgap in most III-V semiconductors. Even so, Si remains the standard material in the electronics industry. A successful combination of these two material systems would add new functionality and increased performance compared to standard Si technology.[1] Although these advantages have long been recognized, the monolithic integration of devicequality III-V materials on Si remains a major challenge. In this work, we report on heteroepitaxial growth of InAs nanowires (NWs) directly on Si substrates by employing self-assembled organic coatings to create an oxide template that guides NW nucleation. Such a template resembles the growth masks used in selective-area epitaxy of nanostructures on III-V substrates. [2][3][4] Importantly, Au, which is commonly used for NW synthesis but not compatible with modern complementary metal oxide semiconductor (CMOS) processing, is avoided. The described nucleation method presents clear advantages in terms of epitaxial quality and control of NW size and density distributions compared to previous results achieved on Si using catalyst-free NW growth. The control demonstrated in the fields of self-assembled [5] and printed organic nanostructures [6,7] illustrates how the method may be extended to more complex patterning in future work. NWs have been the subject of much study and have great potential as a future technology platform. [8,9] One unique feature of the NW geometry is the small NW/substrate interface, which could provide a path to monolithic integration of highperformance materials, such as heterostructure III-V device structures, onto the mainstream Si platform. The small interface helps to mitigate antiphase domain formation, and accommodates a considerable mismatch in lattice constants (ca. 12 % for InAs on Si) and thermal expansion coefficients. [10][11][12] InAs has been used in a number of NW devices (see the literature for examples [13][14][15][16] ), and is one of the most promising materials for high-speed electronics [17] due to its high electron mobility, high electron saturation velocity, and low resistance contacts; still, it has proven difficult to combine InAs directly with Si. At the same time there is a strong drive from the electronics industry to integrate high-performance nanomaterials with Si [1] using methods compatible with existing Si processing. Contamination from the commonly used Au particles in the vapor-liquid-solid (VLS) mechanism [18] for NW growth is a concern because Au is an impurity in Si, which traps electrons and holes by deep-level recombination centers. [19] Inevitably, some traces of Au will contaminate process equipment or end up in the nanostructures grown. [20,21] For this reason, Au is not compatible with modern CMOS processing. NW growth without foreign metal catalyst particles thus offers an attractive alternative to the VLS method. Approaches such...