The surface enhanced Raman spectroscopy (SERS) substrates were fabricated by many methods including the AAO molding and high-cost nanolithography-etching-deposition process. In this article, we have demonstrated the SERS substrate fabricated with silver nanoparticles (Ag-NP) electroless deposition on highly ordered dense hexagonal arrays of UV curable resin nanorods (R-NR) arrays which was reproducible from a precisely controlled anodic aluminum oxide (AAO) template. This method could improve the non-flatness induced defect problem in the conventional nanoimprinting technique and form high-quality duplications of nanometer templates. The periodic hierarchical double-structured nanorods arrays with small nanorods (diameter about 30∼40 nm) in large nanorods (diameter about 100∼110 nm) were obtained by the UV curable resins molding from the AAO template. Two kinds of electroless deposition i.e. self-assembly and ultrasonic vibration methods were performed for Ag-NP formation on R-NR. The enhancement factors of SERS using 10 −5 M methylene blue (MB) as probing molecules were 10 4 ∼10 6 for the self-assembled method and 10 5 ∼10 7 for the ultrasonic vibration one, respectively. This was because the ultrasonic vibration deposition could result in Ag nanorods arrays with higher regularity and contact area than the self-assembly one. A variety of methods have been used to fabricate metallic, ceramic and polymer nanostructures due to the rapid growth of nanofabrication technology that can be classified into two basic categories of top-down and bottom-up approaches. The top-down approaches such as photolithography, 1 focus ion beam, 2 and nanoimprint 3 offered high fidelity and high controllability in terms of design and prediction. However, top-down approaches were generally low throughput and needed expensive instruments. On the other hand, the bottom-up approaches based on self-assembly, such as nanosphere lithography, 4,5 and block copolymer lithography 6 could produce high resolution nanostructures over a large area at low cost but it was difficult to obtain highly uniform and controllable structures of arbitrary symmetries across the whole area. Surface enhanced Raman spectroscopy (SERS) was a useful analytic technique in the food, 4,7,8 chemical molecules, 9,10 and ion detection 11 applications which could provide the detailed information of materials under investigation at the molecular level. The areas with greatly enhanced electromagnetic field became "hot spots" for SERS 12,13 which utilized the field enhancement property of metal nanostructures to amplify the normally weak Raman scattering signals. Different materials and structures were investigated to use as SERS substrates. The preparation of metallic nanostructures with superior SERS performances was one of the main topics in the SERS field and important for sensing and analysis. Currently, SERS have drawn more attentions and made great progress using nanotechnology. Different geometry of nanoflowers 14,15 and nanoparticles 16,17 were used to enhance Raman...