Surface-enhanced Raman scattering (SERS) is a widely used analytical tool that allows molecular fingerprint-based ultra-sensitive detection through an enhanced electromagnetic field generated by plasmonic metal nanoparticles (MNPs) by virtue of their localized surface plasmon resonance (LSPR). Although significant progress has been made in the design and fabrication of a variety of SERS substrates, MNP-decorated electrospun nanofibrous (NF) mats have attracted much attention due to their unique nanoscale structural and functional properties. This review focuses on the current state of the art in the fabrication of plasmonic NF mats with the main focus on the pre-mix, in situ, and ex situ approaches. The characteristic functional advantages and limitations of these strategies are also highlighted, which might be helpful for the research community when adopting a suitable approach. The potential of these plasmonic NF mats as a SERS-active optical sensor substrate, and their performance parameters such as the limit of detection, analytical range, and enhancement factor, and real-world applications are also discussed. The summary and futuristic discussion in this review might be of significant value in developing plasmonic NF mat-based SERS-active point-of-care diagnostic chips for a wide range of applications.