The depletion of good-quality phosphate resources, coupled by a need to supply acceptable products at a rapid rate, while meeting the specifications of fertilizer chemical plants, is of significant concern to the phosphate industry, particularly the production of concentrates with tolerable dolomite content. Tremendous efforts have been made in the past to develop an efficient and economical process that can effectively reject dolomite. However, dolomite removal continues to plague the phosphate industry due to several process-specific challenges being encountered with various beneficiation technologies. In this regard, detailed characterization of phosphate reserves is crucial to understand textural limitations and help design appropriate strategies to achieve quality products. In this paper, the development of procedures to establish dolomite rejection/francolite recovery curves for gravity preconcentration of pebble phosphate from Central Florida is described using high-speed X-ray computed tomography (HSXCT). The developed procedure is illustrated with the analysis of high MgO pebble phosphate samples (10.39 mm × 1 mm) received from South Pasture and Four Corners locations operated by the Mosaic company. The rejection/recovery curves were calculated for each sample for five different particle size classes to observe the trend in rejection/recovery with variation in particle size. In order to evaluate the reliability of the HSXCT data, analysis using the high-resolution X-ray computed tomography (HRXCT) technique was performed on one particular sample (FC-3-1). Finally, to assess the separation efficiency, the HSXCT and HRXCT rejection/recovery curves obtained were compared to experimental gravity preconcentration results reported in the literature. In this way, liberation limitations for gravity preconcentration in the processing of pebble phosphate have been established based on X-ray computed tomography analysis.