Metal-organic frameworks (MOFs), built from organic linkers and metal ions/clusters, have emerged as highly promising materials for wide applications. Combining highly porous crystalline MOFs with the surface-enhanced Raman scattering (SERS) technique can achieve unprecedented advantages of high selectivity, high sensitivity, and expedience in analysis and detection. In this critical review, the aim is to present a comprehensive review of recent advances in understanding of the roles of MOFs in MOF-SERS systems, particularly their structure-to-property correlation. Key examples are selected from representative literature to illustrate critical concepts and the MOFbased property-dependent applications are particularly emphasized. Finally, the barriers, future trends, and prospects for further advances in MOF-SERS platforms are also discussed.