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The Earth Observing-1 (EO-1) satellite was launched on November 21, 2000, as part of a one-year technology demonstration mission. The mission was extended because of the value it continued to add to the scientific community. EO-1 has now been operational for more than a decade, providing both multispectral and hyperspectral measurements. As part of the EO-1 mission, the Advanced Land Imager (ALI) sensor demonstrates a potential technological direction for the next generation of Landsat sensors. To evaluate the ALI sensor capabilities as a precursor to the Operational Land Imager (OLI) onboard the Landsat Data Continuity Mission (LDCM, or Landsat 8 after launch), its measured top-of-atmosphere (TOA) reflectances were compared to the well-calibrated Landsat 7 (L7) Enhanced Thematic Mapper Plus (ETM+) and the Terra Moderate Resolution Imaging Spectroradiometer (MODIS) sensors in the reflective solar bands (RSB). These three satellites operate in a near-polar, sun-synchronous orbit 705 km above the Earth’s surface. EO-1 was designed to fly one minute behind L7 and approximately 30 minutes in front of Terra. In this configuration, all the three sensors can view near-identical ground targets with similar atmospheric, solar, and viewing conditions. However, because of the differences in the relative spectral response (RSR), the measured physical quantities can be significantly different while observing the same target. The cross-calibration of ALI with ETM+ and MODIS was performed using near-simultaneous surface observations based on image statistics from areas observed by these sensors over four desert sites (Libya 4, Mauritania 2, Arabia 1, and Sudan 1). The differences in the measured TOA reflectances due to RSR mismatches were compensated by using a spectral band adjustment factor (SBAF), which takes into account the spectral profile of the target and the RSR of each sensor. For this study, the spectral profile of the target comes from the near-simultaneous EO-1 Hyperion data over these sites. The results indicate that the TOA reflectance measurements for ALI agree with those of ETM+ and MODIS to within 5% after the application of SBAF.