The development of individualized treatments for cancer can be facilitated by more efficient methods for separating cancer cells from patient blood in such a way that they remain viable for live cell assays. We have previously shown that immobilized P-selectin protein can be used on the inner surface of a microscale flow system to induce leukemic cells and leukocytes to roll at different velocities and relative fluxes, thereby creating a means for rapid cell fractionation without inflicting cellular damage. In this study, we explore a method to more efficiently capture leukemic and epithelial cancer cells from flow by altering the nanoscale topography of the inner surface of P-selectin-coated microtubes. This functionalized topography is achieved by attaching naturally occurring halloysite nanotubes to the microtube surface via a monolayer of poly-L-lysine), followed by functionalization with recombinant human selectin protein. We have found that halloysite nanotube coatings promote increased capture of leukemic cells and have determined the key parameters for controlling cell capture under flow: halloysite content and selectin density. Ultimately, selectin-functionalized nanotube coatings should provide a means for enhanced cancer cell isolation from whole blood and other mixtures of cells.