Addition of an amendment or reagent to soil/sediment is a technique that can decrease mobility and reduce bioavailability of uranium (U) and other heavy metals in the contaminated site. According to data from literature and results obtained in field studies, the general mineral class of apatites was selected as a most promising amendment for in situ immobilization/remediation of U. In this work we presented theoretical assessment of stability of U(VI) in four apatite systems (hydroxyapatite (HAP), North Carolina Apatite (NCA), Lisina Apatite (LA), and Apatite II) in order to determine an optimal apatite soil amendment which could be used for in situ remediation of uranium. In this analysis we used a theoretical criterion which is based on calculation of the ion-ion interaction potential, representing the main term of the cohesive energy of the matrix/pollutant system. The presented results of this analysis indicate (i) that the mechanism of immobilization of U by natural apatites depends on their chemical composition and (ii) that all analyzed apatites represent, from the point of view of stability, promising materials which could be used in field remediation of U-contaminated sites.