Hexagonal close-packed tilted Ag nanorod arrays that exhibit excellent uniformity and reproducibility were prepared. The tilt angle was easily controlled by regulating the sputtering angle, accompanied by a reduction and constancy in the gap size of adjacent nanorods, which is 30° and 90° relative to the sputtering direction. The surface enhanced Raman spectroscopy (SERS) technique was used to characterize the interaction of tilted Ag nanorod arrays with polarized laser excitation. Interestingly, the SERS polarization-dependence increased with increasing tilt angle of the Ag nanorods. To elucidate the essential factors responsible for this SERS result, three-dimensional (3D) electromagnetic enhancement distribution for the proposed system was numerically simulated based on p- and s-polarization excitation. Most importantly, the fundamental reasons for the polarization dependence of SERS were obtained by a quantitative 3D numerical simulation of hotspot distribution for adjacent nanorods.