The spectroscopy of aerosols is developing into an active and important field. It allows us to characterize aerosols in a nonintrusive way, in real time, and on site. Understanding the spectroscopic features of these highly complex systems requires the development of novel experimental as well as theoretical methods. This review focuses on infrared extinction spectra. The main goal is to summarize how information about intrinsic particle properties (such as size, shape, and architecture) can be gathered from observed spectroscopic patterns. We discuss the limitations of standard continuum approaches, which have been used for decades to analyze infrared spectra, and we demonstrate the importance of molecular models for the analysis of spectroscopic data.