Sphenopterid specimens from the Late Pennsylvanian of Sydney Coalfield, Canada, are investigated by FTIR and py-GC-MS techniques as part of an on-going research project into the biochemistry and chemotaxonomy of Pennsylvanian-age pteridophylls. Included in the investigation are samples of the true-fern species Oligocarpia brongniartii and Zeilleria delicatula that are preserved as naturally macerated cuticles (NMC), and the seed-fern Eusphenopteris neuropteroides that is also preserved as a compression/impression. FTIR spectra of NMC seed-fern E. neuropteroides, and fern sphenopterid O. brongniartii are very similar, except that the latter does not have aromatic bands in the 700-900 cm-1 out-of-plane region, py-GC-MS show more aromatic compounds for the seed fern than for the two true-fern sphenopterids. Another difference between seed-fern and true-fern sphenopterids is a lower ratio of CH2 to CH3 in chemically treated specimens (CTC) for the seed fern. These observations suggest slightly higher aromaticity for the seed ferns, perhaps related to some chemotaxonomic differences. Comparison of FTIR and py-GC-MS characteristics of sphenopterids and other plant groups shows that these two techniques have potential to identifying chemotaxonomic signals from Carboniferous pteridophylls in general, although more data are needed to confirm this. ?? 2002 Elsevier Science B.V. All rights reserved.