The sensitivity of fluorescent SWCNT-based sensors has been shown to strongly depend on sensor brightness, with the brightest sensors demonstrating enhanced sensitivity capable of single-molecule detection. Although defect-free nanotubes show improved brightness that can enhance sensor sensitivity, the applicability of these nanotubes are often limited by their availability and the sensor preparation procedure, which can introduce defects that diminish quantum yield. Sensor brightness can be tuned to a certain degree through the non-covalent functionalization of SWCNTs with various single-stranded DNA (ssDNA) sequences. However, the correlation between sequence identity and SWCNT brightness remains elusive, and an empirical approach must thus be used to improve brightness. Here, we present a systematic approach to modulating SWCNT brightness through chemical modification of DNA. These modifications can be applied to nearly any DNA sequence, allowing one to enhance SWCNT brightness without significantly altering the sequence-based specificity conferred by the DNA wrapping.