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Testbed (NAST) consists of two passive collocated cross-track scanning instruments, an infrared interferometer (NAST-I) and a microwave radiometer (NAST-M), that fly onboard high-altitude aircraft such as the NASA ER-2 at an altitude near 20 km. NAST-I provides relatively high spectral resolution (0.25-cm⫺1) measurements in the 645–2700-cm⫺1 spectral region with moderate spatial resolution (a linear resolution equal to 13% of the aircraft altitude at nadir) cross-track scanning. We report the methodology for retrieval of atmospheric temperature and composition profiles from NAST-I radiance spectra. The profiles were determined by use of a statistical eigenvector regression algorithm and improved, as needed, by use of a nonlinear physical retrieval algorithm. Several field campaigns conducted under varied meteorological conditions have provided the data needed to verify the accuracy of the spectral radiance, the retrieval algorithm, and the scanning capabilities of this instrumentation. Retrieval examples are presented to demonstrate the ability to reveal fine-scale horizontal features with relatively high vertical resolution.