Our review covers the use of substrates that combine MOFs and metallic nanostructures for SERS -based detection of VOCs in three main contexts: environmental and industrial monitoring, early disease detection through breath analysis, and emerging field of sensing aromas and flavors profiling. Such broad range of application areas underscores the versatility, robustness, and potential of serving in future commercially viable analytical technologies. However, several challenges remain to be solved in order to harness the attractive features of MOF-based SERS substrates and capitalize on the already performed research. In particular, the preparation means suitable for scaling up needs to be established without compromising the well-defined and reproducible plasmonic and chemical features endowed to the substrates. Moreover, developing tools for a systematic selection of the appropriate MOF-substrate pair are needed, taking into account the particular (set of) target analytes, suitable amplification mechanism, and adsorption capacity of the porous framework, not only in terms of surface area but also pore accessibility and pore chemistry. Depending on the application, the platform should be able to analyze patterns in concentration changes of analytes and provide -ideally-with a result at two different levels: identification and quantification of the target analyte(s). This performance characteristics holds potential to advance diseases diagnostics and similarly, may impact newly developing fields of aroma and taste profiling and thus shifting the paradigm of mimicking the sense of smell and taste.