A fully aqueous, N-methyl-2-pyrrolidone–free strategy for debundling single-walled carbon nanotubes (SWCNTs) is reported using the renewable dispersant Vanisperse® LI. Dispersions at 2 mg mL−1 were subjected to probe ultrasonication at 0.3 W mL−1 and evaluated using oscillatory rheology. Complex viscosity (η*) exhibited a transient maximum (~75 min) consistent with the formation of a percolated fibrous network, followed by a decline as debundling progressed. An optimum dispersant coverage of ~1.5 mg m−2 minimized η*, while overdosing likely induced multilayer adsorption and bridging seen by a rapid increase in η*. A two-stage centrifugation at 10,000× g yielded storage-stable suspensions of debundled SWCNTs without ultracentrifugation. SEM confirmed substantial debundling into thin fiber-like bundles. By formulating a dispersion with a dispersant that has a significantly lower cradle-to-gate carbon footprint than both fossil-based and bio-based alternatives such as CMC, this work presents a more sustainable approach to producing debundled SWCNT dispersions for advanced material applications.