Highly ordered arrays of vertically aligned Au-nanotubes (Au-NTs) grafted with radial flocky Au/Ag-nanospikes are fabricated by a combinatorial process of ordered porous anodic aluminum oxide (AAO) template-assisted electrodeposition of Au-NT arrays, wet-chemical removal of AAO, and aniline co-reduction of HAuCl4 and AgNO3 to grow Au/Ag-nanospikes on each Au-NT. As abundant “hot spots” are created uniformly among the gaps between the Au/Ag-nanospikes, the ordered arrays demonstrate highly active and reproducible surface-enhanced Raman scattering effect. Additionally, as this approach can be easily extended to a wide variety of materials, many similar structures of other materials could be achieved for various applications.