A scanning angle total internal reflection (SATIR) Raman spectrometer has been developed for measuring interfacial phenomena with chemical specificity and high axial resolution perpendicular to the interface. The instrument platform is an inverted optical microscope with added automated variable angle optics to control the angle of an incident laser on a prism/sample interface. These optics include two motorized translation stages, the first containing a focusing lens and the second a variable angle galvanometer mirror. The movement of all instrument components is coordinated to ensure that the same sample location and area are probed at each angle. At angles greater than the critical angle, an evanescent wave capable of producing Raman scatter is generated in the sample. The Raman scatter is collected by a microscope objective and directed to a dispersive spectrometer and charge-coupled device detector. In addition to the collected Raman scatter, light reflected from the prism/sample interface is collected to provide calibration parameters that enable modeling the distance over which the Raman scatter is collected for depth profiling measurements. The developed instrument has an incident angle range of 25.5°–75.5°, with a 0.05° angle resolution. Raman scatter can be collected from a ZnSe/organic interface over a range of roughly 35–180 nm. Far from the critical angle, the achieved axial resolution perpendicular to the focal plane is approximately 34 nm. This is roughly a 30-fold improvement relative to confocal Raman microscopy.