Surface-enhanced Raman spectroscopy (SERS) is a highly promising analytical technique that has been widely applied in health and environment monitoring. As a vibrational spectroscopic tool, its fingerprint spectrum contains abundant molecular information, and the greatly enhanced signal can be used to detect analytes at extremely low concentration, even down to the single molecule level. Because water molecules give very weak Raman response, Raman spectroscopy has also been applied for in situ monitoring of targets in solution. However, the Raman signal of an analyte could only be enhanced when it is in proximity to the SERS substrate, which enhances the signal depending on the shape, size, and orientation of the particles constituting the substrate. Further, when using the method for the detection of various analytes, it is necessary to functionalize the SERS substrates, with recognition ligands and encapsulation with a suitable shell among others. Hence, the fabrication of suitable substrates is a basic step in SERS-related research. Tremendous effort has been expended in the last decade in this area, resulting in the development of substrates with unique properties. In this review, we will introduce recent achievements in SERS substrate fabrication based on their structural features. Synthesized nanoparticles, two-dimensional planar substrates, and three-dimensional substrates with effective volume will be discussed in the context of their synthesis strategies along with their characteristic properties. In the future, with further improvement in SERS substrates, the applicability of SERS for detecting a range of analytes in complex environment will become possible.