A simple method for improving surface-enhanced Raman scattering (SERS) performance of aligned silver nanorod (Ag NR) array was investigated. This method was to construct a kind of hybrid substrate by grafting Au@Ag core-shell nanoparticles (NPs) into Ag NR array using poly (2-vinylphridine) (P2VPy) as a bridging agent. The hybrid substrate yielded excellent SERS performance as its detection limit improved from 10 À6 M to 10 À8 M using trans-1,2-bis(4-pyridyl) ethylene (BPE) as probe molecule, which was increased by two orders of magnitude compared with Ag NR array substrate. The signi¯cant improvement of SERS performance of Ag NR arrays was attributed to the addition of Au@Ag core-shell NPs. As a result of surface plasmon resonance generated by the interaction of electromagnetic (EM) (IAEM)¯led between NP and NR structures, increasing hotspots were found at the connections of NPs and NRs, the gaps of adjacent rods, and the gaps of two particles consequently. These results were validated by the¯nite di®erence time domain (FDTD) calculation. Besides, hybrid substrate shows good performance in stability and reproducibility. The proposed method was simple and robust, which promoted SERS performance of Ag NR array e®ectively, showing great potential in the application of SERS substrate fabrication and SERS-based bio-chemical sensing.