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The interaction of 23 gases and solvents with the basal plane of highly oriented pyrolytic graphite (HOPG) and with single-wall carbon nanotube (SWCNT) samples is studied using thermal desorption spectroscopy. Pre-exponential frequency factors used for analysis of desorption traces are obtained from vapor pressure data. Activation energies for desorption at monolayer coverage are determined using the Redhead peak-maximum method. Binding energies of non-polar adsorbates to the HOPG surface are found to scale with the adsorbate polarizability providing clear evidence for the van der Waals character of the interaction. Low coverage desorption temperatures on SWCNT samples are found to be 50–100% higher than on HOPG. Such increase has previously been attributed to physisorption in higher coordinated sites such as grooves on the external SWCNT rope surfaces. Polar adsorbates on the other hand typically desorb at much higher temperatures from SWCNT samples which is here tentatively attributed to stronger interaction with defect sites.