We report the manufacture of ordered silver and copper nanorod arrays for surface-enhanced Raman scattering using oblique angle deposition (OAD) on prepatterned polymer sheets. It was found that the patterned polymer substrate defined nucleation sites which guided subsequent growth of nanorods. Enhanced surface-enhanced Raman spectroscopy (SERS) intensities of the Raman probe molecule trans-1,2-bis(4-pyridyl)ethylene (BPE) were found for Ag arrays on polymer, up to about 10 times that of the Ag–silica control. The SERS response of Ag nanorod arrays of different structures was investigated alongside results obtained from discrete dipole approximation simulations. This revealed that narrow gaps between nanorods, formed by guided nucleation during OAD, were responsible for this dramatic enhancement. Ordered Cu nanorod arrays were also successfully fabricated, producing a SERS intensity about 3 times that of Cu on silicon for both BPE and another Raman probe—rhodamine B isothiocyanate (RBITC)—highlighting the potential of this large-scale, low-cost, SERS-active substrate.