Vibrational spectroscopy techniques provide a powerful approach to the study of environmental materials and processes. These multifunctional analytical tools can be used to probe molecular vibrations of solid, liquid, and gaseous samples for characterizing materials, elucidating reaction mechanisms, and examining kinetic processes. Although Fourier transform infrared (FTIR) spectroscopy is the most prominent type of vibrational spectroscopy used in the field of soil science, applications of Raman spectroscopy to study environmental samples continue to increase. The ability of FTIR and Raman spectroscopies to provide complementary information for organic and inorganic materials makes them ideal approaches for soil science research. In addition, the ability to conduct in situ, real time, vibrational spectroscopy experiments to probe biogeochemical processes at mineral interfaces offers unique and versatile methodologies for revealing a myriad of soil chemical phenomena. This review provides a comprehensive overview of vibrational spectroscopy techniques and highlights many of the applications of their use in soil chemistry research.