Analyses of identifiable organic fossil remains of animals and plants have considerable potential to resolve conflicting models of organic matter diagenesis and kerogen formation (e.g. selective preservation versus random polymerization). Fossil cuticles of arthropods (scorpion, eurypterid) and plants (cordaite, pteridosperm) from Upper Carboniferous strata of Lone Star Lake, Kansas, USA and Joggins, Nova Scotia, Canada were analysed by pyrolysis–gas chromatography/mass spectrometry and examined by electron microscopy. Recent Pandinus (scorpion) and Araucaria (conifer) provided a basis for comparison. Pyrolysis of Recent dewaxed scorpion cuticle yielded products derived from chitin and proteins. These products were absent in the fossil arthropod cuticles, however, which yielded an homologous series of alkanes and alkenes, together with phenolic and other aromatic constituents. Recent dewaxed plant cuticle yielded fatty acids, phenols and carbohydrate-derived compounds indicative of cutin polyester and associated lignocellulose. The pyrolysates of the fossil plant cuticles, on the other hand, were dominated by alkane–alkene doublets, with minor phenolic and other benzenoid components. There is no evidence that the preservation of these cuticles as particulate organic matter in kerogen is simply a result of selective preservation. Nonetheless, the chemistry and morphology remain characteristic of a particular taxon, thereby eliminating the possibility of incorporation of randomly repolymerized materials or the transfer of material between plant and animal residues. The aliphatic moieties in the fossil cuticles are thought to be the result of polymerization of the associated epicuticular, cuticular and/or tissue lipids during diagenesis.