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In recent years, there has been a significant increase in the use of remotely sensed data to address global issues. With the open data policy, the data from the Moderate Resolution Imaging Spectroradiometer (MODIS) and Enhanced Thematic Mapper Plus (ETM+) sensors have become a critical component of numerous applications. These two sensors have been operational for more than a decade, providing a rich archive of multispectral imagery for analysis of mutitemporal remote sensing data. This paper focuses on evaluating the radiometric calibration agreement between MODIS and ETM+ using the near-simultaneous and cloud-free image pairs over an African pseudo-invariant calibration site, Libya 4. To account for the combined uncertainties in the top-of-atmosphere (TOA) reflectance due to surface and atmospheric bidirectional reflectance distribution function (BRDF), a semiempirical BRDF model was adopted to normalize the TOA reflectance to the same illumination and viewing geometry. In addition, the spectra from the Earth Observing-1 (EO-1) Hyperion were used to compute spectral corrections between the corresponding MODIS and ETM+ spectral bands. As EO-1 Hyperion scenes were not available for all MODIS and ETM+ data pairs, MODerate resolution atmospheric TRANsmission (MODTRAN) 5.0 simulations were also used to adjust for differences due to the presence or lack of absorption features in some of the bands. A MODIS split-window algorithm provides the atmospheric water vapor column abundance during the overpasses for the MODTRAN simulations. Additionally, the column atmospheric water vapor content during the overpass was retrieved using the MODIS precipitable water vapor product. After performing these adjustments, the radiometric cross-calibration of the two sensors was consistent to within 7%. Some drifts in the response of the bands are evident, with MODIS band 3 being the largest of about 6% over 10 years, a change that will be corrected in Collection 6 MODIS processing.