The challenge of assembling semiconducting single-wall carbon nanotubes (s-SWCNTs) into densely packed, aligned arrays has limited the scalability and practicality of high-performance nanotube-based electronics technologies. The aligned deposition of s-SWCNTs via floating evaporative self-assembly (FESA) has promise for overcoming this challenge; however, the mechanisms behind FESA need to be elucidated before the technique can be improved and scaled. Here, we gain a deeper understanding of the FESA process by studying a stationary analogue of FESA and optically tracking the dynamics of the organic ink/water/substrate and ink/air/substrate interfaces during the typical FESA process. We observe that the ink/water interface serves to collect and confine the s-SWCNTs before alignment and that the deposition of aligned bands of s-SWCNTs occurs at the ink/water/substrate contact line during the depinning of both the ink/air/substrate and ink/water/substrate contact lines. We also demonstrate improved control over the interband spacing, bandwidth, and packing density of FESA-aligned s-SWCNT arrays. The substrate lift rate (5-15 mm min(-1)) is used to tailor the interband spacing from 90 to 280 mu m while Maintaining a constant aligned s-SWCNT bandwidth of 50 mu m. Varying the s-SWCNT ink concentration (0.75-10 mu g mL(-1)) allows the control of the bandwidth from 2.5 to 45 mu m. A steep increase in packing density is observed from 11 s-SWCNTs mu m(-1) at 0.7 mu g mL(-1) to 20 s-SWCNTs mu m(-1) at 2 mu g mL(-1), with a saturated packing density of similar to 24 s-SWCNTs mu m(-1). We also demonstrate the scaling of FESA to align s-SWCNTs on a 2.5 X 2.5 cm(2) scale while preserving high-quality alignment on the nanometer scale. These findings help realize the scalable fabrication of well-aligned s-SWCNT arrays to serve as large-area platforms for next-generation semiconductor electronics.