Lanthanum-modified bentonite (LMB, commercially called Phoslock®) has been widely applied in freshwater systems to manage eutrophication. Little is known, however, about its behaviour and efficiency in binding filterable reactive phosphorus (FRP) in saline environments. We assessed if LMB would adsorb phosphate over a range of salinities (0–32 ppth) comparing the behaviour in seawater salts and equivalent concentrations of NaCl. Lanthanum release from the bentonite matrix was measured and the La species prevailing in saline environments were evaluated through chemical equilibrium modelling. We demonstrated that LMB was able to adsorb FRP in all the salinities tested. Filterable lanthanum (FLa) concentrations were similarly low (<5 μgL−1) at all seawater salinities but considerably elevated, on occasion >2000 times greater in equivalent NaCl salinities. Mineralogical analysis indicates that La present in the clay interlayer was (partially) replaced by Na/Ca/Mg present in the seawater and a possible secondary P-reactive phase was formed, such as kozoite (LaCO3OH) or lanthanite (La2(CO3)3·8H2O) that may be physically dissociated from the LMB. Geochemical modelling also indicates that most FLa dissociated from LMB would be precipitated as a carbonate complex. In light of the identification of reactive intermediate phases, further studies including ecotoxicologial assays are required to assess any deleterious effects from the application of LMB to saline waters.