Escherichia coli (E. coli) is a well-established indicator of faecal pollution and a potent pathogen linked to numerous gastrointestinal and systemic illnesses. Ensuring public safety requires rapid and sensitive detection methods capable of real-time, on-site deployment. Many conventional techniques are either laborious, time-intensive, costly, or require complex infrastructure, limiting their applicability in field settings. Raman spectroscopy offers label-free molecular fingerprinting; however, its inherently weak scattering signals restrict its effectiveness as a standalone technique. Surface-Enhanced Raman Spectroscopy (SERS) overcomes this limitation by exploiting plasmonic enhancement from nanostructured metallic substrates—most commonly gold, silver, copper, and aluminium. Despite the commercial availability of SERS-active substrates, challenges remain in achieving high reproducibility, long-term stability, and true field applicability, necessitating the development of integrated lab-on-chip platforms and portable, handheld Raman devices. This review critically examines recent advances in SERS-based E. coli detection across water and perishable food products with particular emphasis on the evolution of SERS substrate design, the incorporation of biosensing elements, and the integration of electrochemical and microfluidic systems. By contrasting conventional SERS approaches with next-generation biosensing strategies, this paper outlines pathways toward robust, real-time pathogen detection technologies suitable for both laboratory and field applications.