Oils and asphaltenes are generally assumed to be key intermediates in coal liquefaction. Since fundamental chemical/ mathematical principles require compositionally unique fractions, mass spectrometry and infrared spectroscopy were employed to obtain detailed molecular analyses of fractionated coal-liquid-derived oils and asphaltenes. The asphaltenes contain higher molecular weight homologs in many specific-Z series and different compound types than do the oils. However, both fractions contain appreciable quantities of compound types equivalent in molecular formula and, hence, assumably in molecular structure. The chemical/physical properties of oils and asphaltenes are not describable in terms of average (hypothetical) molecular structures. The lack of unique oil and asphaltene compositions necessitates detailed molecular analysis as a prerequisite for understanding, assessing, and controlling the chemical/physical phenomena intrinsic to production and processing of coal liquids.T he concept of preasphaltenes, asphaltenes, and oils is of historical significance in the development of the science and technology of coal liquefaction (J). This concept is routinely employed in attempts to understand, assess,