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The implementation of the Climate Absolute Radiance and Refractivity Observatory (CLARREO) mission was recommended by the National Research Council in 2007 to provide an on-orbit intercalibration standard with accuracy of 0.3% (k = 2) for relevant Earth observing sensors. The goal of reference intercalibration, as established in the Decadal Survey, is to enable rigorous high-accuracy observations of critical climate change parameters, including reflected broadband radiation [Clouds and Earth's Radiant Energy System (CERES)], cloud properties [Visible Infrared Imaging Radiometer Suite (VIIRS)], and changes in surface albedo, including snow and ice albedo feedback. In this paper, we describe the CLARREO approach for performing intercalibration on orbit in the reflected solar (RS) wavelength domain. It is based on providing highly accurate spectral reflectance and reflected radiance measurements from the CLARREO Reflected Solar Spectrometer (RSS) to establish an on-orbit reference for existing sensors, namely, CERES and VIIRS on Joint Polar Satellite System satellites, Advanced Very High Resolution Radiometer and follow-on imagers on MetOp, Landsat imagers, and imagers on geostationary platforms. One of two fundamental CLARREO mission goals is to provide sufficient sampling of high-accuracy observations that are matched in time, space, and viewing angles with measurements made by existing instruments, to a degree that overcomes the random error sources from imperfect data matching and instrument noise. The data matching is achieved through CLARREO RSS pointing operations on orbit that align its line of sight with the intercalibrated sensor. These operations must be planned in advance; therefore, intercalibration events must be predicted by orbital modeling. If two competing opportunities are identified, one target sensor must be given priority over the other. The intercalibration method is to monitor changes in targeted sensor response function parameters: effective - ffset, gain, nonlinearity, optics spectral response, and sensitivity to polarization. In this paper, we use existing satellite data and orbital simulation methods to determine mission requirements for CLARREO, its instrument pointing ability, methodology, and needed intercalibration sampling and data matching for accurate intercalibration of RS radiation sensors on orbit. We conclude that with the CLARREO RSS in a polar 90° inclination orbit at a 609-km altitude, estimated intercalibration sampling will limit the uncertainty contribution from data matching noise to 0.3% (k = 2) over the climate autocorrelation time period. The developed orbital modeling and intercalibration event prediction will serve as a framework for future mission operations.