peer reviewed ; Major and trace element (Rb, Sr, Ba, Zr, Ni, V, Zn, Cr, Y, Ce) compositions are studied in Lower Devonian terrigenous sediments from the Dinant Synclinorium and Ardenne Anticline (Belgian Ardenne). Five cross sections encompassing 148 samples in 19 formations have been studied. In the conventional [Al2O3+Fe2O3-K2O-Na2O]–[K2O]–[FeO+MgO] triangle, the rock compositions plot on the illite – chlorite tie line. This suggests that (1) the mineral association has reached equilibrium in the pressure and temperature range of the postdepositional evolution of the sediments; (2) the chemical system was open and K was a mobile component. Although the original composition of the sediment was modified, the AAFM = Al2O3/Al2O3+FeOt+MgO parameter that reflects the illite - chlorite proportions can be used as a proxy of the source composition. A principal component analysis of the major and trace element compositions permits to define the behaviour of various elements currently used as proxies of various processes. Noteworthy it is shown that Ti, V and part of Cr are correlated with the illite proportion, and part of Cr, together with Zr, with resistate minerals such as quartz, chromite and zircon. The evolution with stratigraphic age in the 5 cross sections of the AAFM proxy reveals that there is a major change in the northern part of the Ardenne Anticline at the limit between the Mirwart Formation and younger formations, corresponding approximately to the Lochkovian to Pragian transition. There is a clear shift from an aluminium-rich source to a more conventional chlorite-rich source. In the paleogeographic evolution of this region the only possible source of the aluminium-rich sediment is the Rocroi Massif. Our results confirm sedimentological and palynological evidence that a “Rocroi Island” existed in the Lochkovian Sea. A decrease in Zr concentrations with distance to the Rocroi Massif also supports this hypothesis. The stratigraphic evolution of several parameters shows local variations that can be ...