Sorption processes on mineral surfaces are a critical factor in controlling the distribution and accumulation of potentially harmful metals in the environment. This work investigates the effectiveness of gypsum (CaSO4⋅2H2O) to sequester Pb. The interaction of gypsum fragments with Pb-bearing solutions (10, 100 and 1000mg/L) was monitored by performing macroscopic batch-type experiments conducted at room temperature. The aqueous phase composition was periodically determined by Atomic Absorption Spectrometry (AAS), Ion Chromatography (IC) and Inductively Coupled Plasma Optical Emission Spectroscopy (ICP–OES). Regardless of the [Pbaq]initial, a [Pbaq]final <4mg/L was always reached. The uptake process was fast (t <1h) for [Pbaq]initial ⩾100mg/L and significantly slower (t >1week) for [Pbaq]initial =10mg/L. Speciation calculations revealed that after a long time of interaction (1month), all the solutions reached equilibrium with respect to both gypsum and anglesite. For [Pbaq]initial ⩾100mg/L, sorption takes place mainly via the rapid dissolution of gypsum and the simultaneous formation of anglesite both on the gypsum surface and in the bulk solution. In the case of [Pbaq]initial =10mg/L, no anglesite precipitation was observed, but surface spectroscopy (proton Rutherford Backscattering Spectroscopy, p-RBS) confirmed the formation of Pb-bearing surface layers on the (010) gypsum surface in this case also. This study shows that the surface of gypsum can play an important role in the attenuation of Pb in contaminated waters.