Column-averaged dry-air mole fractions of carbon dioxide (XCO2) and methane (XCH4) measured by a solar viewing portable Fourier transform spectrometer (FTS, EM27/SUN) have been characterized and validated by comparison using in situ profile measurements made during the transfer flights of two aircraft campaigns: Korea-United States Air Quality Study (KORUS-AQ) and Effect of Megacities on the Transport and Transformation of Pollutants at Regional and Global Scales (EMeRGe). The aircraft flew over two Total Carbon Column Observing Network (TCCON) sites: Rikubetsu, Japan (43.46∘ N, 143.77∘ E), for the KORUS-AQ campaign and Burgos, Philippines (18.53∘ N, 120.65∘ E), for the EMeRGe campaign. The EM27/SUN was deployed at the corresponding TCCON sites during the overflights. The mole fraction profiles obtained by the aircraft over Rikubetsu differed between the ascending and the descending flights above approximately 8 km for both CO2 and CH4. Because the spatial pattern of tropopause heights based on potential vorticity values from the ERA5 reanalysis shows that the tropopause height over the Rikubetsu site was consistent with the descending profile, we used only the descending profile to compare with the EM27/SUN data. Both the XCO2 and XCH4 derived from the descending profiles over Burgos were lower than those from the ascending profiles. Output from the Weather Research and Forecasting Model indicates that higher CO2 for the ascending profile originated in central Luzon, an industrialized and densely populated region about 400 km south of the Burgos TCCON site. Air masses observed with the EM27/SUN overlap better with those from the descending aircraft profiles than those from the ascending aircraft profiles with respect to their properties such as origin and atmospheric residence times. Consequently, the descending aircraft profiles were used for the comparison with the EM27/SUN data. The EM27/SUN XCO2 and XCH4 data were derived by using the GGG2014 software without applying air-mass-independent correction factors (AICFs). The comparison of the EM27/SUN observations with the aircraft data revealed that, on average, the EM27/SUN XCO2 data were biased low by 1.22 % and the EM27/SUN XCH4 data were biased low by 1.71 %. The resulting AICFs of 0.9878 for XCO2 and 0.9829 for XCH4 were obtained for the EM27/SUN. Applying AICFs being utilized for the TCCON data (0.9898 for XCO2 and 0.9765 for XCH4) to the EM27/SUN data induces an underestimate for XCO2 and an overestimate for XCH4.