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The ordered Ag nanorod (AgNR) arrays are fabricated through a simple electroless deposition technique using the isolated Si nanowire (SiNW) arrays as the Ag-grown scaffold. The AgNR arrays have the single-crystallized structure and the plasmonic crystal feature. It is found that the formation of the AgNR arrays is strongly dependent on the filling ratio of SiNWs. A mechanism is proposed based on the selective nucleation and the synergistic growth of Ag nanoparticles on the top of the SiNWs. Moreover, the special AgNR arrays grown on the substrate of SiNWs exhibit a detection sensitivity of 10−15M for rhodamine 6G molecules, which have the potential application to the highly sensitive surface-enhanced Raman scattering sensors.