The high demand for thin, lightweight yet fast and efficient devices is a driving force behind the miniaturization trend in the electronics industry. Specifically, the advancement of semiconducting single-walled carbon nanotubes (SWNTs) can continue to revolutionize transistors, although there are still many challenges ahead. We have previously reported an alignment relay technique (ART) that is capable of simultaneously controlling the alignment, length, and diameter of surface deposited SWNTs. However, the current technique yields inconsistencies in orientation, lengths of tubes, and their density. Here, we present a reviewed ART protocol that includes sonication for improved selectivity. We show that the SWNTs average alignment increased from 40% to 77% within a 10°range in orientation with sonication times as low as 5 min. Sonication generated larger diameter nanotubes on the surface, with a preference for semiconducting chiral tubes in the range of 1.44−1.61 nm in diameter. Consequently, simple alterations to the standard alignment relay technique can prove to be prosperous in improving selectivity and orientational control of single-walled carbon nanotubes. This work has direct impact for the simultaneous control of nanotube alignment and nanotube chiralities.