High blood cholesterol levels increase the risk of heart disease, which is the leading cause of death in the United States. Current interventions for high cholesterol include pharmaceuticals such as statins, which have considerable negative side effects, and expensive apheresis treatment in severe cases of hypercholesterolemia. To remove cholesterol from serum, we use digitonin bound to single-wall carbon nanotubes (SWCNTs). Digitonin is a nonionic, biological surfactant that specifically binds to cholesterol, but previous studies with digitonin required extensive ultracentrifugation to separate the digitonin/cholesterol complex. We have found that digitonin also has the ability to noncovalently bind to SWCNTs and individually disperse them in water. We characterized SWCNTs-digitonin dispersions using ultraviolet-visible-near infrared (UV-vis-NIR) absorbance, NIR fluorescence, and Raman spectroscopies. Our results show that digitonin dispersed SWCNTs individually in water at any SWCNT:digitonin weight ratio greater than 1:2, and the dispersions remained stable for more than 2 months. SWCNTs provide a structural component and high surface area-to-volume ratio to anchor digitonin molecules while simultaneously binding to cholesterol. We removed any free digitonin from SWCNT-digitonin dispersions and then added them to cholesterol-containing serum. SWCNTs-digitonin agglomerated upon binding to cholesterol within 24 hours while remaining individualized within the agglomerate; SWCNT aggregation state was monitored using the aforementioned spectroscopic techniques. These SWCNTs-digitonin-cholesterol agglomerates, which removed ≈ 46 wt% of serum cholesterol measured using an enzymatic fluorescent assay, could be readily decanted from the remaining serum. We use a thermodynamic model of binding to suggest that digitonin will show similar interactions with other graphitic structures while simultaneously binding to cholesterol, allowing for development of an in-line filter from free-standing graphitic porous structures to remove cholesterol from blood.