The Montevive celestine mineral deposit, set in the Granada Basin in a marine evaporitic uppermost Tortonian–lowermost Messinian sequence, is the largest reserve in Europe of this economically important strontium ore. Currently, the mine has a large amount of tailings resulting from the rejection of a manual dry screening of high-grade celestine mineral. This visual and density screening was carried out in the early days of mining (1954–1973). Concentrating the celestine mineral and increasing the ore recovery rate would reduce mine operation costs and the generation of new tailings, reducing the impact on the environment. In order to define more adequate concentration methods, we have used complementary analytical techniques such as optical (OM) and scanning and transmission electron microscopy (SEM and TEM), energy-dispersive X-rays (EDXs), X-ray fluorescence (XRF), and X-ray diffraction (XRD) to fully characterize the morphology, microstructure, chemistry, and mineralogy of the celestine mineral. The low-grade mineral is made of prismatic celestine crystals that are replacing a matrix of micro sparry calcite. Other minority minerals are strontianite, dolomite, quartz, and clays (kaolinite, paragonite, and illite). There is also a certain amount of iron oxides and hydroxides (mainly magnetite) associated with clays. We showed that the concentration of low-grade celestine mineral can be achieved through a low-cost and eco-friendly method based on grinding and size separation. The coarser fractions (>5 mm) have more celestine (up to 12 percent units higher than the starting unprocessed mineral) due to the selective loss of calcite and minority minerals (quartz, clays, and iron oxides) that are mainly found in the finer fraction (<1 mm). This process can make mine exploitation more sustainable, reducing the generation of residues that negatively impact the environment.