Knowledge of the binding mechanisms of heavy metals to cement minerals is essential for the prediction of the long-term leachability of secondary building materials and cement-stabilized wastes containing heavy metals. In this study, the sorption of Zn(II) to calcium silicate hydrate (C-S-H(I)) in pre-equilibrated aqueous suspensions has been investigated as a function of time (up to 87 d), pH (11.7, 12.48, and 12.78) and Zn(II) concentration (4.8-4800 microM). Electron probe microanalysis (EPMA) was performed in order to determine where Zn(II) was bound. At high Zn(II) concentrations (>1000 microM), the precipitation of beta2-Zn-(OH)2 (< pH 12) and calcium zincate (Zn2Ca(OH)6 x 2H2O, > pH 12) was observed. Surface precipitation could not be discerned. At lower concentrations, it was found that the sorption process was initially very rapid with over 50% sorbed within 30 min but that the sorption continued more slowly to at least 87 d. The data could be interpreted in terms of the Freundlich isotherm up to a Si:Zn(II)sorbed atomic ratio of approximately 6:1. Zinc was observed by EPMA to incorporate into the C-S-H(I) particles but did not appear to substitute for Ca or Si. The incorporation of Zn(ll) in the interlayer of C-S-H(I) or sorption to internal surfaces of crystalline appear to be the most probable mechanisms for the observed Zn(II) sorption to C-S-H(I).