Surface-enhanced Raman scattering (SERS) is one of the most promising sensing techniques as it is non-invasive, non-destructive, and can reveal the spectral “fingerprints” of molecules. However, it remains a great challenge to fabricate large-scale, highly reproducible SERS substrates. In this work, we have developed a novel method to fabricate a long-range, highly ordered, plasmonic gold nano-ring array pattern based on a modified nanosphere lithography technique. The optical properties of gold nanoring array have been comprehensively studied and optimized for SERS by tuning the geometric parameters of the nanoring arrays using a combination of finite-difference time-domain (FDTD) simulations and cleanroom fabrication techniques. The optimized gold nanoring array has been further demonstrated for SERS biosensing.