This report describes a validation study of Greenhouse gases Observing Satellite (GOSAT) data processing using ground-based measurements of the Total Carbon Column Observing Network (TCCON) as reference data for column-averaged dry air mole fractions of atmospheric carbon dioxide (X_(CO_2)). We applied the photon path length probability density function method to validate X_(CO_2) retrievals from GOSAT data obtained during 22 months starting from June 2009. This method permitted direct evaluation of optical path modifications due to atmospheric light scattering that would have a negligible impact on ground-based TCCON measurements but could significantly affect gas retrievals when observing reflected sunlight from space. Our results reveal effects of optical path lengthening over Northern Hemispheric stations, essentially from May–September of each year, and of optical path shortening for sun-glint observations in tropical regions. These effects are supported by seasonal trends in aerosol optical depth derived from an offline three-dimensional aerosol transport model and by cirrus optical depth derived from space-based measurements of the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument. Removal of observations that were highly contaminated by aerosol and cloud from the GOSAT data set resulted in acceptable agreement in the seasonal variability of XCO2 over each station as compared with TCCON measurements. Statistical comparisons between GOSAT and TCCON coincident measurements of CO_2 column abundance show a correlation coefficient of 0.85, standard deviation of 1.80 ppm, and a sub-ppm negative bias of −0.43 ppm for all TCCON stations. Global distributions of monthly mean retrieved X_(CO_2) with a spatial resolution of 2.5° latitude × 2.5° longitude show agreement within ∼2.5 ppm with those predicted by the atmospheric tracer transport model.