This dissertation revisits, develops, and documents methods that can be used to calibrate spaceborne microwave radiometers once in orbit. The on-orbit calibration methods discussed within this dissertation can provide accurate and early results by utilizing Calibration Attitude Maneuvers (CAM), which encompasses Deep Space Calibration (DSC) and a new use of the Second Stokes (SS) analysis that can provide early and much needed insight on the performance of the instrument. This dissertation describes pre-existing and new methods of using DSC maneuvers as well as a simplified use of the SS procedure. Over TRMM's 17 years of operation it has provided invaluable data and has performed multiple CAMs over its lifetime. These maneuvers are analyzed to implement on-orbit calibration procedures that will be applied for future missions. In addition, this research focuses on the radiometric calibration of TMI that will be incorporated in the final processing (Archive/Legacy of the NASA TMI 1B11 brightness temperature data product). This is of importance since TMI's 17-year sensor data record must be vetted of all known calibration errors so to provide the final stable data for science users, specifically, climatological data records.