This study presents a new conceptual approach to estimate total column mole fractions of CO2 and CH4 using partial column data. It provides a link between airborne in situ and remote sensing observations of greenhouse gases. The method relies on in situ observations, external ancillary sources of information (e.g., atmospheric transport models), and a regression kriging framework. We evaluate our new approach using National Oceanic and Atmospheric Administration's (NOAA's) AirCore program-in situ vertical profiles of CO2 and CH4 collected from weather balloons. Our paper shows that under the specific conditions of this study and assumption of unbiasedness, airborne observations up to 6500-9500maltitude are required to achieve comparable total column CO2 mole fraction uncertainty as the Total Carbon Column Observing Network (TCCON) network provides, given as a precision of the ratio between observed and true total column-integrated mole fraction, assuming 400 ppm XCO2 (2σ, e.g., 0.8 ppm). If properly calibrated, our approach could be applied to vertical profiles of CO2 collected from aircraft using a few flask samples, while retaining similar uncertainty level. Our total column CH4 estimates, by contrast, are less accurate than TCCON's. Aircrafts are not as spatially constrained as TCCON ground stations, so our approach adds value to aircraft-based vertical profiles for evaluating remote sensing platforms.