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The demonstration of a newly developed compact thermal imager (CTI) on the International Space Station (ISS) has provided not only a technology advancement but a rich high-resolution dataset on global clouds, atmospheric and land emissions. This study showed that the free-running CTI instrument could be calibrated to produce scientifically useful radiance imagery of the atmosphere, clouds, and surfaces with a vertical resolution of ~460 m at limb and a horizontal resolution of ~80 m at nadir. The new detector demonstrated an excellent sensitivity to detect the weak limb radiance perturbations modulated by small-scale atmospheric gravity waves. The CTI’s high-resolution imaging was used to infer vertical cloud temperature profiles from a side-viewing geometry. For nadir imaging, the combined high-resolution and high-sensitivity capabilities allowed the CTI to better separate cloud and surface emissions, including those in the planetary boundary layer (PBL) that had small contrast against the background surface. Finally, based on the ISS’s orbit, the stable detector performance and robust calibration algorithm produced valuable diurnal observations of cloud and surface emissions with respect to solar local time during May–October 2019, when the CTI had nearly continuous operation.