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Remote Sensing Group (RSG) at the University of Arizona has a long history of using ground-based test sites for the calibration of airborne- and satellite-based sensors. Often, ground-truth measurements at these tests sites are not always successful due to weather and funding availability. Therefore, RSG has also employed automated ground instrument approaches and cross-calibration methods to verify the radiometric calibration of a sensor. The goal in the cross-calibration method is to transfer the calibration of a well-known sensor to that of a different sensor.This dissertation presents a method for determining the radiometric calibration of a hyperspectral imager using multispectral imagery. The work relies on a multispectral sensor, Moderate-resolution Imaging Spectroradiometer (MODIS), as a reference for the hyperspectral sensor Hyperion. Test sites used for comparisons are Railroad Valley in Nevada and a portion of the Libyan Desert in North Africa. A method to predict hyperspectral surface reflectance using a combination of MODIS data and spectral shape information is developed and applied for the characterization of Hyperion. Spectral shape information is based on RSG's historical in situ data for the Railroad Valley test site and spectral library data for the Libyan test site. Average atmospheric parameters, also based on historical measurements, are used in reflectance prediction and transfer to space. Results of several cross-calibration scenarios that differ in image acquisition coincidence, test site, and reference sensor are found for the characterization of Hyperion. These are compared with results from the reflectance-based approach of vicarious calibration, a well-documented method developed by the RSG that serves as a baseline for calibration performance for the cross-calibration method developed here. Cross-calibration provides results that are within 2% of those of reflectance-based results in most spectral regions. Larger disagreements exist for shorter wavelengths studied in this work as well as in spectral areas that experience absorption by the atmosphere.