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Abstract To exploit their charge transport properties in transistors, semiconducting carbon nanotubes must be assembled into aligned arrays comprised of individualized nanotubes at optimal packing densities. However, achieving this control on the wafer‐scale is challenging. Here, solution‐based shear in substrate‐wide, confined channels is investigated to deposit continuous films of well‐aligned, individualized, semiconducting nanotubes. Polymer‐wrapped nanotubes in organic ink are forced through sub‐mm tall channels, generating shear up to 10 000 s−1uniformly aligning nanotubes across substrates. The ink volume and concentration, channel height, and shear rate dependencies are elucidated. Optimized conditions enable alignment within a ±32° window, at 50 nanotubes µm−1, on 10 × 10 cm2substrates. Transistors (channel length of 1–5 µm) are fabricated parallel and perpendicular to the alignment. The parallel transistors perform with 7× faster charge carrier mobility (101 and 49 cm2V−1s−1assuming array and parallel‐plate capacitances, respectively) with high on/off ratio of 105. The spatial uniformity varies ±10% in density, ±2° in alignment, and ±7% in mobility. Deposition occurs within seconds per wafer, and further substrate scaling is viable. Compared to random networks, aligned nanotube films promise to be a superior platform for applications including sensors, flexible/stretchable electronics, and light emitting and harvesting devices.more » « less
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