Two approaches to producing gradients of vertically aligned single-walled carbon nanotubes (SWCNTs) on silicon surfaces by chemical grafting are presented here. The first approach involves the use of a porous silicon (pSi) substrate featuring a pore size gradient, which is functionalized with 3-aminopropyltriethoxysilane (APTES). Carboxylated SWCNTs are then immobilized on the topography gradient via carbodiimide coupling. Our results show that as the pSi pore size and porosity increase across the substrate the SWCNT coverage decreases concurrently. In contrast, the second gradient is an amine-functionality gradient produced by means of vapor-phase diffusion of APTES from a reservoir onto a silicon wafer where APTES attachment changes as a function of distance from the APTES reservoir. Carboxylated SWCNTs are then immobilized via carbodiimide coupling to the amine-terminated silicon gradient. Our observations confirm that with decreasing APTES density on the surface the coverage of the attached SWCNTs also decreases. These gradient platforms pave the way for the time-efficient optimization of SWCNT coverage for applications ranging from field emission to water filtration to drug delivery.