Synthesis, characterization and sorption affinities of titanium phosphate (TiP) and titanium phosphate silicates (TiPSi) in relation to various metal ions were recently reported by our group. In this work, we explored further adsorption properties of these materials with respect to aluminium ions in aqueous solutions. Sorption of Al3+(aq) increases with pH and reaches ca. 13 mg/g at pH close to neutral conditions and it can be described by an ion-exchange mechanism. Surface speciation of aluminium was studied by 27Al and 31P solid state NMR. These and other spectroscopic data were correlated with adsorption macroscopic measurements. Purification of process and drinking waters is one of the potential applications of these cheap adsorbents manufactured by decomposition of mineral sphene, CaTiOSiO4, which is abundant up to 5 % in tailings of apatite ores in Kola peninsula.