This work presents elemental composition studies of human dental calculus by X-ray fluorescence analysis using synchrotron radiation. The intrinsic characteristics of synchrotron light allow for a quantitative analysis of major, minor, and trace elements of very small samples in a single measurement. At present, several theories of calculus formation exist, but none of them can describe completely all the complicated mechanisms involved in the mineralization processes. For this reason, and taking into account that experimental data are long overdue, several calculi with certain degrees of formation were collected from adult patients for analysis. The ratio of calcium/phosphorus was used as an indicator of the major crystalline structure and the state of formation of the calculus. The results demonstrate a clear correlation between the concentrations of certain elements and the type of calculus (supra- or sub-gingival). In addition, the possible correlation between the elements was analyzed.