This data set contains pyrolysis gas composition resulting from experimental fires in longleaf pine fuel beds burned in a wind tunnel and in small experimental fires at Ft. Jackson, SC. The gases were sampled and then measured by Fourier Transform Infrared (FTIR) spectroscopy. These data were collected from the same experiments contained in the "Pyrolysis gases measured by gas chromatography and mass spectrometry from fires in a wind tunnel and at Ft. Jackson, SC" data set and many of the data files and metadata in that product describe the locations, fuels, environmental conditions and fire behavior information related to this data product. The wind tunnel data spectra were captured in real time using both static (composite sample) and dynamic (time-series) modes; the Ft. Jackson data were collected in canisters and processed offline within a day of collection. A total of 29 gases were identified including small alkanes, alkenes, aldehydes, nitrogen compounds, and aromatics, most previously measured by FTIR in wildland fires. A total of 33 static (23 wind tunnel and 10 field) and 10 dynamic (wind tunnel) samples were analyzed. Wind tunnel gas concentration data estimated using external cavity quantum cascade lasers are also included. The pyrolysis gas composition in this data set, in combination with the data product "Pyrolysis gases measured by gas chromatography and mass spectrometry from fires in a wind tunnel and at Ft. Jackson, SC", were compared with the pyrolysis gas composition determined using traditional methods contained in the data product "Pyrolysis gases produced by fast and slow pyrolysis of foliage samples from 15 plants common to the southeastern US coastal plain". The use of trade or firm names is for information and does not imply endorsement by the US Department of Agriculture of any product or service.