The use of carbon-based nanomaterials to improve the sensitivity of surface-enhanced Raman spectroscopy (SERS) for the detection of contaminants has been reviewed in this chapter. Because of its high sensitivity, specificity, and potential for label-free detection of various chemical pollutants, SERS has become a potent analytical tool in response to the growing need for quick, sensitive environmental, and food safety monitoring detection techniques. Reduced graphene oxide (rGO), carbon nanotubes (CNTs), carbon quantum dots (CQDs), and carbon nanofibers (CNFs) are examples of carbon nanomaterials that are useful SERS substrates because of their special physicochemical characteristics, which include chemical stability, high surface area, and tunable electronic characteristics. Specifically, hybrid nanocomposites that combine metallic nanoparticles like gold (Au) or silver (Ag) with carbon nanomaterials provide synergistic enhancements through chemical and electromagnetic mechanisms, enabling detection limits for various environmental contaminants. This chapter also examines the potential of carbon nanomaterials in next-generation monitoring technologies for thorough contaminant profiling and future directions for their integration in scalable, environmentally friendly SERS platforms. Case studies showing the sensitive and selective detection of priority pollutants in complex matrices highlight the effectiveness of different carbon-based SERS platforms. With the promise of easily accessible applications in industrial and environmental settings, special attention is paid to developing portable SERS devices that use carbon-based substrates for on-site testing. These developments position carbon nanomaterial-enhanced SERS as a game-changing method for accurate, real-time contaminant detection in various fields.