Phosphate (Pi) sequestration by a lanthanum (La) exchanged clay mineral (La-Bentonite), which is extensively used in chemical lake restoration, was investigated on the molecular level using a combination of 31P and 139La solid state NMR spectroscopy (SSNMR), extended X-ray absorption spectroscopy (EXAFS) and powder X-ray diffraction (PXRD) and sorption studies. 31P SSNMR show that all phosphate was immobilized as rhabdophane (LaPO4·n H2O, n  3), which was further supported by 139La SSNMR and EXAFS. However, PXRD results were ambiguous with respect to rhabdophane and monazite (LaPO4). Adsorption studies showed that at dissolved organic carbon (DOC) concentration above ca. 250 M the binding capacity was only 50 % of the theoretical value or even less. No other La or Pi phases were detected by SSNMR and EXAFS indicating the effect of DOC is kinetic. Moreover, 31P SSNMR showed that rhabdophane formed upon Pi sequestration is in close proximity to the clay matrix.