The Advanced Technology Microwave Sounder (ATMS) is a passive microwave radiometer for the current generation of polar-orbiting meteorological satellites operated by the National Oceanic and Atmospheric Administration (NOAA). The first two ATMS instruments are manifested onboard the Suomi National Polar-orbiting Partnership (S-NPP) and NOAA-20 satellites. Several critical changes have been made to ATMS operational calibration algorithm since March 2017. The calibration processing has been revised from a Rayleigh–Jeans approximated algorithm to a full radiance algorithm in order to reduce the error introduced by the approximation over cold radiances in the higher frequency channels. In addition, based on the lessons learned from S-NPP and NOAA-20 postlaunch calibration/validation tests, some major improvements have been made in the updated operational algorithm. These include reflector emission and antenna pattern corrections. Details of the radiance-based ATMS on-orbit calibration are documented in this report, and results of prelaunch calibration error budget analysis and postlaunch calibration accuracy evaluation are also presented for reference.