As a way to control the surface properties of nanowires and nanotubes, we present a method for growing polymer from the surface of silicon/silica core/shell nanowires. After modification of nanowire surfaces with polymer initiators, Atom Transfer Radical Polymerization (ATRP) was used to grow methacrylate polymer chains from the surface. The resulting structures were characterized by SEM, TEM, and EELS. After etching the silicon cores, the resulting polymer-coated nanotubes will have hydrophilic silica cores with hydrophobic polymer shells.