Seacoal and gilsonite are used by the foundry industry as carbonaceous additives in green molding sands. In this study, pyrolysis was used to simulate the heating conditions that the carbonaceous additives would experience during metal casting. Gas chromatography-mass spectrometry was used to tentatively identify major organic products generated during their pyrolysis at 500, 750, and 1000 degrees C. A number of compounds of environmental concern were identified during the pyrolysis of seacoal and gilsonite, including substituted benzenes, phenolics, and polycyclic aromatic hydrocarbons (PAHs). These thermal decomposition products, and especially PAHs, were generated at each pyrolysis temperature in all foundry sands containing seacoal. In gilsonite-amended sand, however, mainly alkanes and alkenes were identified at 500 and 750 degrees C and PAHs at 1000 degrees C. Compared to seacoal, the most intense peaks occurred during the pyrolysis of sand containing gilsonite. The greatest loss of pyrolyzable material also occurred during heating of gilsonite-amended sand from ambient temperature to 1000 degrees C in a thermogravimetric analyzer. The results obtained from this study will be useful to green sand foundries looking to reduce volatile hydrocarbon emissions. Published by Elsevier B. V.