High-performance liquid chromatography (HPLC) based techniques are used to investigate the role of polar species in deposit formation during jet fuel autoxidation and to explore the relative contributions of the various species classes which compose the polar fraction. More specifically, HPLC with UV-vis absorption detection was employed to quantify the polar species in jet fuel as a class, and a technique which combines solid-phase extraction (SPE) with HPLC and gas chromatography with mass spectrometric detection (GC-MS) was used to identify the species classes which compose the polar fraction in typical jet fuels. The analytical results were combined with surface deposit data obtained in a quartz crystal microbalance (QCM) system for a series of twenty jet fuels. The results indicate a relationship between the total amount of polar species measured and the amount of surface deposits produced. Results also suggest that phenols, various other oxygenated polar species, indoles, and carbazoles have a significant positive correlation with jet fuel surface deposit formation, while pyridines, anilines, and quinolines do not demonstrate a strong correlation with the tendency of a fuel to form surface deposits.